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We report the synthesis of graphene/fullerene-capped gold nanoparticle nanocomposite film which was used to construct supercapacitor electrodes. The fullerene-based self-assembled monolayers on gold nanoparticles (AuNPs) were attained via the fullerene(C60)-gold interaction. The fullerene-capped AuNPs effectively separated the graphene sheets preventing aggregation. A synergistic effect was observed—the specific capacitance of graphene/fullerene-capped AuNP electrode is197 F/g, which is higher than that of graphene electrode (31 F/g), graphene/AuNP electrode (126 F/g), and graphene/fullerene electrode (118 F/g). The results render a novel route of synthesis and modification of graphene-based materials for the construction of electrochemical energy storage devices.