The cyanometallic framework (CMF)-derived bimetallic oxide/graphene foam (GF) composites were synthesized by a solution immersion and subsequent annealing treatment. As a binder-free electrode for supercapacitors, the Co3O4-NiO/GF electrode exhibited remarkable electrochemical properties in terms of high specific capacity (766 F g−1 at 1 A g−1), superior rate capability with 67% capacitance retention (0.5–10 A g−1), as well as excellent cycling stability (86% retention after 5000 cycles). The improved capacitance performances were ascribed to the strong synergistic interaction between hierarchical Co3O4-NiO and GF substrate, where metal oxides contributed to high pseudocapacitance and GF provided outstanding conductivity and structural stability of electrodes.