Abstract: Graphite owning low cost, high stability, and low voltage platform has been regarded as the preferred commercial anode material in lithium batteries （LIBs）. However, the graphite anode is prone to expansion, exfoliation, and pulverization during a long-term charge and discharge process in LIBs, thereby leading to poor cycling and rate performance. To solve the above problems, designing new-type structures in graphite has become the main method to improve its lithium-ion storage performance. Herein, this work integrates air pre-oxidation with introducing trace high valence metal chloride of AlCl₃ intercalation agent to regulate the microstructure in flake graphite, including interlayer spacing, crystallinity, defect degree and C=O content. To well investigate the microstructure changes of the modified graphite （GOAl）, some characterization techniques including XRD, XPS, Raman, BET and TEM have been employed to fabricate the relationships between various microstructures of GOAl and lithium-ion storage performance, and thus revealing the lithium-ion storage mechanism to effectively establish a controllable preparation technology of high-performance graphite anode materials in LIBs. It has been demonstrated that this modification strategy can expand the carbon interlayer spacing, introduce rich C=O groups and defect structures, thereby effectively enhance the specific capacity, rate performance and cycling stability of graphite anode. The modified graphite anode exhibits a specific capacity of 357.55 mAh/g at 0.1 C （1 C=372 mA/g）, and still delivers a high specific capacity of 267 mAh/g at 2 C after 200 cycles. The reaction kinetics of GOAl anode have been analyzed by using GITT, dQ/dV and EIS. These results demonstrate that the GOAl anode has a faster lithium-ion diffusion rate, lower polarization voltage and smaller charge transfer impedance compared with pure graphite. These improved electrochemical properties of graphite anode can be ascribed to the enhanced interlayer spacing, abundant C=O groups and defect structures in GOAl, which can effectively reduce the binding energy between solvated Li⁺ with C to facilitate Li⁺ de-solvation process, meanwhile increases lithium-ion storage room.