diff --git a/python/ray/tests/test_placement_group.py b/python/ray/tests/test_placement_group.py
index fd292f124..348e5e9cc 100644
--- a/python/ray/tests/test_placement_group.py
+++ b/python/ray/tests/test_placement_group.py
@@ -1178,7 +1178,7 @@ def test_create_placement_group_after_gcs_server_restarts(
 
     # Create placement group 1 successfully.
     placement_group1 = ray.util.placement_group([{"CPU": 1}, {"CPU": 1}])
-    ray.get(placement_group1.ready(), timeout=2)
+    ray.get(placement_group1.ready(), timeout=10)
     table = ray.util.placement_group_table(placement_group1)
     assert table["state"] == "CREATED"
 
@@ -1188,7 +1188,7 @@ def test_create_placement_group_after_gcs_server_restarts(
 
     # Create placement group 2 successfully.
     placement_group2 = ray.util.placement_group([{"CPU": 1}, {"CPU": 1}])
-    ray.get(placement_group2.ready(), timeout=2)
+    ray.get(placement_group2.ready(), timeout=10)
     table = ray.util.placement_group_table(placement_group2)
     assert table["state"] == "CREATED"
 
@@ -1253,7 +1253,7 @@ def test_create_placement_group_during_gcs_server_restart(
     cluster.head_node.start_gcs_server()
 
     for i in range(0, 10):
-        ray.get(placement_groups[i].ready(), timeout=2)
+        ray.get(placement_groups[i].ready())
 
 
 if __name__ == "__main__":
diff --git a/src/ray/gcs/gcs_server/gcs_placement_group_manager.cc b/src/ray/gcs/gcs_server/gcs_placement_group_manager.cc
index 74d95e82a..1028b6337 100644
--- a/src/ray/gcs/gcs_server/gcs_placement_group_manager.cc
+++ b/src/ray/gcs/gcs_server/gcs_placement_group_manager.cc
@@ -470,6 +470,7 @@ void GcsPlacementGroupManager::LoadInitialData(const EmptyCallback &done) {
   auto callback = [this,
                    done](const std::unordered_map<PlacementGroupID,
                                                   rpc::PlacementGroupTableData> &result) {
+    std::unordered_map<NodeID, std::vector<rpc::Bundle>> node_to_bundles;
     for (auto &item : result) {
       auto placement_group = std::make_shared<GcsPlacementGroup>(item.second);
       if (item.second.state() != rpc::PlacementGroupTableData::REMOVED) {
@@ -479,9 +480,20 @@ void GcsPlacementGroupManager::LoadInitialData(const EmptyCallback &done) {
             item.second.state() == rpc::PlacementGroupTableData::RESCHEDULING) {
           pending_placement_groups_.emplace_back(std::move(placement_group));
         }
+
+        if (item.second.state() == rpc::PlacementGroupTableData::CREATED ||
+            item.second.state() == rpc::PlacementGroupTableData::RESCHEDULING) {
+          const auto &bundles = item.second.bundles();
+          for (auto &bundle : bundles) {
+            node_to_bundles[NodeID::FromBinary(bundle.node_id())].emplace_back(bundle);
+          }
+        }
       }
     }
 
+    // Notify raylets to release unused bundles.
+    gcs_placement_group_scheduler_->ReleaseUnusedBundles(node_to_bundles);
+
     SchedulePendingPlacementGroups();
     RAY_LOG(INFO) << "Finished loading initial data.";
     done();
diff --git a/src/ray/gcs/gcs_server/gcs_placement_group_scheduler.cc b/src/ray/gcs/gcs_server/gcs_placement_group_scheduler.cc
index 58e12d213..5dc85a047 100644
--- a/src/ray/gcs/gcs_server/gcs_placement_group_scheduler.cc
+++ b/src/ray/gcs/gcs_server/gcs_placement_group_scheduler.cc
@@ -204,6 +204,17 @@ void GcsPlacementGroupScheduler::ScheduleUnplacedBundles(
     std::shared_ptr<GcsPlacementGroup> placement_group,
     std::function<void(std::shared_ptr<GcsPlacementGroup>)> failure_callback,
     std::function<void(std::shared_ptr<GcsPlacementGroup>)> success_callback) {
+  // We need to ensure that the PrepareBundleResources won't be sent before the reply of
+  // ReleaseUnusedBundles is returned.
+  if (!nodes_of_releasing_unused_bundles_.empty()) {
+    RAY_LOG(INFO) << "Failed to schedule placement group " << placement_group->GetName()
+                  << ", id: " << placement_group->GetPlacementGroupID() << ", because "
+                  << nodes_of_releasing_unused_bundles_.size()
+                  << " nodes have not released unused bundles.";
+    failure_callback(placement_group);
+    return;
+  }
+
   auto bundles = placement_group->GetUnplacedBundles();
   auto strategy = placement_group->GetStrategy();
 
@@ -556,6 +567,34 @@ GcsPlacementGroupScheduler::GetBundlesOnNode(const NodeID &node_id) {
   return bundles_on_node;
 }
 
+void GcsPlacementGroupScheduler::ReleaseUnusedBundles(
+    const std::unordered_map<NodeID, std::vector<rpc::Bundle>> &node_to_bundles) {
+  // The purpose of this function is to release bundles that may be leaked.
+  // When GCS restarts, it doesn't know which bundles it has scheduled in the
+  // previous lifecycle. In this case, GCS will send a list of bundle ids that
+  // are still needed. And Raylet will release other bundles. If the node is
+  // dead, there is no need to send the request of release unused bundles.
+  const auto &alive_nodes = gcs_node_manager_.GetAllAliveNodes();
+  for (const auto &alive_node : alive_nodes) {
+    const auto &node_id = alive_node.first;
+    nodes_of_releasing_unused_bundles_.insert(node_id);
+
+    auto lease_client = GetLeaseClientFromNode(alive_node.second);
+    auto release_unused_bundles_callback =
+        [this, node_id](const Status &status,
+                        const rpc::ReleaseUnusedBundlesReply &reply) {
+          nodes_of_releasing_unused_bundles_.erase(node_id);
+        };
+    auto iter = node_to_bundles.find(alive_node.first);
+
+    // When GCS restarts, some nodes maybe do not have bundles.
+    // In this case, GCS will send an empty list.
+    auto bundles_in_use =
+        iter != node_to_bundles.end() ? iter->second : std::vector<rpc::Bundle>{};
+    lease_client->ReleaseUnusedBundles(bundles_in_use, release_unused_bundles_callback);
+  }
+}
+
 void BundleLocationIndex::AddBundleLocations(
     const PlacementGroupID &placement_group_id,
     std::shared_ptr<BundleLocations> bundle_locations) {
diff --git a/src/ray/gcs/gcs_server/gcs_placement_group_scheduler.h b/src/ray/gcs/gcs_server/gcs_placement_group_scheduler.h
index 5baadc6d4..7ccabdc12 100644
--- a/src/ray/gcs/gcs_server/gcs_placement_group_scheduler.h
+++ b/src/ray/gcs/gcs_server/gcs_placement_group_scheduler.h
@@ -74,6 +74,12 @@ class GcsPlacementGroupSchedulerInterface {
   /// \param placement_group_id The placement group id scheduling is in progress.
   virtual void MarkScheduleCancelled(const PlacementGroupID &placement_group_id) = 0;
 
+  /// Notify raylets to release unused bundles.
+  ///
+  /// \param node_to_bundles Bundles used by each node.
+  virtual void ReleaseUnusedBundles(
+      const std::unordered_map<NodeID, std::vector<rpc::Bundle>> &node_to_bundles) = 0;
+
   virtual ~GcsPlacementGroupSchedulerInterface() {}
 };
 
@@ -385,6 +391,12 @@ class GcsPlacementGroupScheduler : public GcsPlacementGroupSchedulerInterface {
   absl::flat_hash_map<PlacementGroupID, std::vector<int64_t>> GetBundlesOnNode(
       const NodeID &node_id) override;
 
+  /// Notify raylets to release unused bundles.
+  ///
+  /// \param node_to_bundles Bundles used by each node.
+  void ReleaseUnusedBundles(const std::unordered_map<NodeID, std::vector<rpc::Bundle>>
+                                &node_to_bundles) override;
+
  protected:
   /// Send a bundle PREPARE request to a node. The PREPARE request will lock resources
   /// on a node until COMMIT or CANCEL requests are sent to a node.
@@ -477,6 +489,9 @@ class GcsPlacementGroupScheduler : public GcsPlacementGroupSchedulerInterface {
   /// Set of placement group that have lease requests in flight to nodes.
   absl::flat_hash_map<PlacementGroupID, std::shared_ptr<LeaseStatusTracker>>
       placement_group_leasing_in_progress_;
+
+  /// The nodes which are releasing unused bundles.
+  absl::flat_hash_set<NodeID> nodes_of_releasing_unused_bundles_;
 };
 
 }  // namespace gcs
diff --git a/src/ray/gcs/gcs_server/test/gcs_placement_group_manager_test.cc b/src/ray/gcs/gcs_server/test/gcs_placement_group_manager_test.cc
index af86eab3d..9f6050ace 100644
--- a/src/ray/gcs/gcs_server/test/gcs_placement_group_manager_test.cc
+++ b/src/ray/gcs/gcs_server/test/gcs_placement_group_manager_test.cc
@@ -40,6 +40,10 @@ class MockPlacementGroupScheduler : public gcs::GcsPlacementGroupSchedulerInterf
 
   MOCK_METHOD1(MarkScheduleCancelled, void(const PlacementGroupID &placement_group_id));
 
+  MOCK_METHOD1(
+      ReleaseUnusedBundles,
+      void(const std::unordered_map<NodeID, std::vector<rpc::Bundle>> &node_to_bundles));
+
   absl::flat_hash_map<PlacementGroupID, std::vector<int64_t>> GetBundlesOnNode(
       const NodeID &node_id) override {
     absl::flat_hash_map<PlacementGroupID, std::vector<int64_t>> bundles;
diff --git a/src/ray/gcs/gcs_server/test/gcs_placement_group_scheduler_test.cc b/src/ray/gcs/gcs_server/test/gcs_placement_group_scheduler_test.cc
index 5e6fb352b..021ccdef4 100644
--- a/src/ray/gcs/gcs_server/test/gcs_placement_group_scheduler_test.cc
+++ b/src/ray/gcs/gcs_server/test/gcs_placement_group_scheduler_test.cc
@@ -1014,6 +1014,13 @@ TEST_F(GcsPlacementGroupSchedulerTest, TestPGCancelledDuringReschedulingCommitPr
   WaitPlacementGroupPendingDone(1, GcsPlacementGroupStatus::FAILURE);
 }
 
+TEST_F(GcsPlacementGroupSchedulerTest, TestReleaseUnusedBundles) {
+  SchedulePlacementGroupSuccessTest(rpc::PlacementStrategy::SPREAD);
+  std::unordered_map<NodeID, std::vector<rpc::Bundle>> node_to_bundle;
+  scheduler_->ReleaseUnusedBundles(node_to_bundle);
+  ASSERT_EQ(1, raylet_clients_[0]->num_release_unused_bundles_requested);
+}
+
 }  // namespace ray
 
 int main(int argc, char **argv) {
diff --git a/src/ray/gcs/gcs_server/test/gcs_server_test_util.h b/src/ray/gcs/gcs_server/test/gcs_server_test_util.h
index c6134e08e..24b71c4ee 100644
--- a/src/ray/gcs/gcs_server/test/gcs_server_test_util.h
+++ b/src/ray/gcs/gcs_server/test/gcs_server_test_util.h
@@ -183,6 +183,12 @@ struct GcsServerMocker {
       return_callbacks.push_back(callback);
     }
 
+    void ReleaseUnusedBundles(
+        const std::vector<rpc::Bundle> &bundles_in_use,
+        const rpc::ClientCallback<rpc::ReleaseUnusedBundlesReply> &callback) override {
+      ++num_release_unused_bundles_requested;
+    }
+
     // Trigger reply to PrepareBundleResources.
     bool GrantPrepareBundleResources(bool success = true) {
       Status status = Status::OK();
@@ -231,6 +237,7 @@ struct GcsServerMocker {
     int num_lease_requested = 0;
     int num_return_requested = 0;
     int num_commit_requested = 0;
+    int num_release_unused_bundles_requested = 0;
     NodeID node_id = NodeID::FromRandom();
     std::list<rpc::ClientCallback<rpc::PrepareBundleResourcesReply>> lease_callbacks = {};
     std::list<rpc::ClientCallback<rpc::CommitBundleResourcesReply>> commit_callbacks = {};
diff --git a/src/ray/protobuf/node_manager.proto b/src/ray/protobuf/node_manager.proto
index 887787cc4..087135e39 100644
--- a/src/ray/protobuf/node_manager.proto
+++ b/src/ray/protobuf/node_manager.proto
@@ -148,6 +148,13 @@ message RequestObjectSpillageReply {
   bool success = 1;
 }
 
+message ReleaseUnusedBundlesRequest {
+  repeated Bundle bundles_in_use = 1;
+}
+
+message ReleaseUnusedBundlesReply {
+}
+
 // Service for inter-node-manager communication.
 service NodeManagerService {
   // Request a worker from the raylet.
@@ -186,4 +193,10 @@ service NodeManagerService {
   // Ask the raylet to spill an object to external storage.
   rpc RequestObjectSpillage(RequestObjectSpillageRequest)
       returns (RequestObjectSpillageReply);
+  // This method is only used by GCS, and the purpose is to release bundles
+  // that may be leaked. When GCS restarts, it doesn't know which bundles it has leased
+  // in the previous lifecycle. In this case, GCS will send a list of bundles that
+  // are still needed. And Raylet will release other bundles.
+  rpc ReleaseUnusedBundles(ReleaseUnusedBundlesRequest)
+      returns (ReleaseUnusedBundlesReply);
 }
diff --git a/src/ray/raylet/node_manager.cc b/src/ray/raylet/node_manager.cc
index a8bf79699..60705cef6 100644
--- a/src/ray/raylet/node_manager.cc
+++ b/src/ray/raylet/node_manager.cc
@@ -558,6 +558,36 @@ void NodeManager::HandleRequestObjectSpillage(
       });
 }
 
+void NodeManager::HandleReleaseUnusedBundles(
+    const rpc::ReleaseUnusedBundlesRequest &request,
+    rpc::ReleaseUnusedBundlesReply *reply, rpc::SendReplyCallback send_reply_callback) {
+  RAY_CHECK(!new_scheduler_enabled_) << "Not implemented";
+  RAY_LOG(DEBUG) << "Releasing unused bundles.";
+  std::unordered_set<BundleID, pair_hash> in_use_bundles;
+  for (int index = 0; index < request.bundles_in_use_size(); ++index) {
+    const auto &bundle_id = request.bundles_in_use(index).bundle_id();
+    in_use_bundles.emplace(
+        std::make_pair(PlacementGroupID::FromBinary(bundle_id.placement_group_id()),
+                       bundle_id.bundle_index()));
+  }
+
+  // TODO(ffbin): Kill all workers that are currently associated with the unused bundles.
+  // At present, the worker does not have a bundle ID, so we cannot filter out the workers
+  // used by unused bundles. We will solve it in next pr.
+
+  // Return unused bundle resources.
+  for (auto iter = bundle_spec_map_.begin(); iter != bundle_spec_map_.end();) {
+    if (0 == in_use_bundles.count(iter->first)) {
+      ReturnBundleResources(*iter->second);
+      bundle_spec_map_.erase(iter++);
+    } else {
+      iter++;
+    }
+  }
+
+  send_reply_callback(Status::OK(), nullptr, nullptr);
+}
+
 // TODO(edoakes): this function is problematic because it both sends warnings spuriously
 // under normal conditions and sometimes doesn't send a warning under actual deadlock
 // conditions. The current logic is to push a warning when: all running tasks are
@@ -1986,6 +2016,8 @@ bool NodeManager::PrepareBundle(
     // Register bundle state.
     bundle_state->state = CommitState::PREPARED;
     bundle_state_map_.emplace(bundle_id, bundle_state);
+    bundle_spec_map_.emplace(
+        bundle_id, std::make_shared<BundleSpecification>(bundle_spec.GetMessage()));
   }
   return bundle_state->acquired_resources.AvailableResources().size() > 0;
 }
diff --git a/src/ray/raylet/node_manager.h b/src/ray/raylet/node_manager.h
index d911155d2..6e7726528 100644
--- a/src/ray/raylet/node_manager.h
+++ b/src/ray/raylet/node_manager.h
@@ -645,6 +645,11 @@ class NodeManager : public rpc::NodeManagerServiceHandler {
                                    rpc::RequestObjectSpillageReply *reply,
                                    rpc::SendReplyCallback send_reply_callback) override;
 
+  /// Handle a `ReleaseUnusedBundles` request.
+  void HandleReleaseUnusedBundles(const rpc::ReleaseUnusedBundlesRequest &request,
+                                  rpc::ReleaseUnusedBundlesReply *reply,
+                                  rpc::SendReplyCallback send_reply_callback) override;
+
   /// Trigger global GC across the cluster to free up references to actors or
   /// object ids.
   void TriggerGlobalGC();
@@ -816,6 +821,10 @@ class NodeManager : public rpc::NodeManagerServiceHandler {
   /// creation.
   absl::flat_hash_map<BundleID, std::shared_ptr<BundleState>, pair_hash>
       bundle_state_map_;
+
+  /// Save `BundleSpecification` for cleaning leaked bundles after GCS restart.
+  absl::flat_hash_map<BundleID, std::shared_ptr<BundleSpecification>, pair_hash>
+      bundle_spec_map_;
 };
 
 }  // namespace raylet
diff --git a/src/ray/raylet_client/raylet_client.cc b/src/ray/raylet_client/raylet_client.cc
index 77c4aff93..e541ee413 100644
--- a/src/ray/raylet_client/raylet_client.cc
+++ b/src/ray/raylet_client/raylet_client.cc
@@ -402,6 +402,25 @@ void raylet::RayletClient::CancelResourceReserve(
   grpc_client_->CancelResourceReserve(request, callback);
 }
 
+void raylet::RayletClient::ReleaseUnusedBundles(
+    const std::vector<rpc::Bundle> &bundles_in_use,
+    const rpc::ClientCallback<rpc::ReleaseUnusedBundlesReply> &callback) {
+  rpc::ReleaseUnusedBundlesRequest request;
+  for (auto &bundle : bundles_in_use) {
+    request.add_bundles_in_use()->CopyFrom(bundle);
+  }
+  grpc_client_->ReleaseUnusedBundles(
+      request,
+      [callback](const Status &status, const rpc::ReleaseUnusedBundlesReply &reply) {
+        if (!status.ok()) {
+          RAY_LOG(WARNING)
+              << "Error releasing bundles from raylet, the raylet may have died:"
+              << status;
+        }
+        callback(status, reply);
+      });
+}
+
 void raylet::RayletClient::PinObjectIDs(
     const rpc::Address &caller_address, const std::vector<ObjectID> &object_ids,
     const rpc::ClientCallback<rpc::PinObjectIDsReply> &callback) {
diff --git a/src/ray/raylet_client/raylet_client.h b/src/ray/raylet_client/raylet_client.h
index 936f6a3c1..8799366a6 100644
--- a/src/ray/raylet_client/raylet_client.h
+++ b/src/ray/raylet_client/raylet_client.h
@@ -118,6 +118,10 @@ class ResourceReserveInterface {
       BundleSpecification &bundle_spec,
       const ray::rpc::ClientCallback<ray::rpc::CancelResourceReserveReply> &callback) = 0;
 
+  virtual void ReleaseUnusedBundles(
+      const std::vector<rpc::Bundle> &bundles_in_use,
+      const rpc::ClientCallback<rpc::ReleaseUnusedBundlesReply> &callback) = 0;
+
   virtual ~ResourceReserveInterface(){};
 };
 
@@ -380,6 +384,11 @@ class RayletClient : public PinObjectsInterface,
       const ray::rpc::ClientCallback<ray::rpc::CancelResourceReserveReply> &callback)
       override;
 
+  /// Implements ReleaseUnusedBundlesInterface.
+  void ReleaseUnusedBundles(
+      const std::vector<rpc::Bundle> &bundles_in_use,
+      const rpc::ClientCallback<rpc::ReleaseUnusedBundlesReply> &callback) override;
+
   void PinObjectIDs(
       const rpc::Address &caller_address, const std::vector<ObjectID> &object_ids,
       const ray::rpc::ClientCallback<ray::rpc::PinObjectIDsReply> &callback) override;
diff --git a/src/ray/rpc/node_manager/node_manager_client.h b/src/ray/rpc/node_manager/node_manager_client.h
index e82c45b7e..1c9b16c18 100644
--- a/src/ray/rpc/node_manager/node_manager_client.h
+++ b/src/ray/rpc/node_manager/node_manager_client.h
@@ -100,6 +100,9 @@ class NodeManagerWorkerClient
   /// Ask the raylet to spill an object to external storage.
   VOID_RPC_CLIENT_METHOD(NodeManagerService, RequestObjectSpillage, grpc_client_, )
 
+  /// Release unused bundles.
+  VOID_RPC_CLIENT_METHOD(NodeManagerService, ReleaseUnusedBundles, grpc_client_, )
+
  private:
   /// Constructor.
   ///
diff --git a/src/ray/rpc/node_manager/node_manager_server.h b/src/ray/rpc/node_manager/node_manager_server.h
index 2db6706eb..08893d49f 100644
--- a/src/ray/rpc/node_manager/node_manager_server.h
+++ b/src/ray/rpc/node_manager/node_manager_server.h
@@ -35,7 +35,8 @@ namespace rpc {
   RPC_SERVICE_HANDLER(NodeManagerService, PrepareBundleResources) \
   RPC_SERVICE_HANDLER(NodeManagerService, CommitBundleResources)  \
   RPC_SERVICE_HANDLER(NodeManagerService, CancelResourceReserve)  \
-  RPC_SERVICE_HANDLER(NodeManagerService, RequestObjectSpillage)
+  RPC_SERVICE_HANDLER(NodeManagerService, RequestObjectSpillage)  \
+  RPC_SERVICE_HANDLER(NodeManagerService, ReleaseUnusedBundles)
 
 /// Interface of the `NodeManagerService`, see `src/ray/protobuf/node_manager.proto`.
 class NodeManagerServiceHandler {
@@ -100,6 +101,10 @@ class NodeManagerServiceHandler {
   virtual void HandleRequestObjectSpillage(const RequestObjectSpillageRequest &request,
                                            RequestObjectSpillageReply *reply,
                                            SendReplyCallback send_reply_callback) = 0;
+
+  virtual void HandleReleaseUnusedBundles(const ReleaseUnusedBundlesRequest &request,
+                                          ReleaseUnusedBundlesReply *reply,
+                                          SendReplyCallback send_reply_callback) = 0;
 };
 
 /// The `GrpcService` for `NodeManagerService`.