Multi-core architectures have been broadly utilized in current processors. Meanwhile, the diversity of memory access modes in applications brings challenges to the last level Cache in multi-core processors. An optimization method for the last level Cache based on the access modes is proposed. This method includes three coordinated and progressive levels:the configurable share/private Cache partition, the configurable bypass Cache policy, and the priority replace policy. Using this method, programmers can neatly alter the behavior of the last level Cache to effectively adapt the variety of memory access modes in applications. Experiment results show that the proposed method can observably decrease the miss rate of the last level Cache and increase the system performance of the processor.