This work explored the effect of graphene surface modification on the electrochemical performance of polyaniline-based nanocomposite. The surface modification of graphene was confirmed by Fourier transform infrared spectroscopy. Field emission scanning electron microscopy and high-resolution transmission electron microscopy showed uniform polyaniline coating of the modified graphene. The specific capacitance of the graphene/polyaniline composite was 242 F/g, but it decreased to 193 F/g after graphene modification. However, the capacitance retention increased from 86% to 89% after 500 cycles due to the graphene modification. The thermal stability of the composite also increased after the graphene modification.