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Flake graphite was mechanically modified at different times in N-methyl pyrrolidone under normal pressure. The results of the scanning electron microscopy, X-ray diffraction, and transmission electron microscopy suggested that the structure of the flake graphite was modified. The crystallinity of the flake graphite, and many defects were introduced into the material. The evaluation of capacitor performance by cyclic voltammetry, galvanostatic charge/discharge tests, and electrochemical impedance spectroscopy was also performed. Results showed that the electrochemical performance of flake graphite was strongly enhanced, particularly when it was exfoliated for 6 h. Moreover, the electrochemical capacitive properties of activated carbon were obviously enhanced through the substitution of acetylene black by flake graphite modified for 6 h.