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Graphene paper (GP) with layered structure and highly conductive network is fabricated by a facile technique of vacuum filtration and studied as a single-component and binder-free anode of lithium ion batteries (LIBs). The process of fabrication of GP without any binder and high-temperature treatment, in the meantime, great improvement in both the capacity and cycling performance of the GP electrodes have compared with other kinds of traditional graphite electrode materials. Given the simplifying anode fabrication, low manufacturing costs and many electrochemical properties of the GP anode, it is regarded as an excellent anode material of LIB with great promise for its both excellent cycling performance and electrochemical properties. The specific capacity can reach to over 200 mAhg-1after 60 charge-discharge cycles under the current rate of 50 mAg-1.