Graphene nanosheets are deposited on nickel foams with 3D porous structure by an electrophoretic deposition method using the colloids of graphene monolayers in ethanol as electrolytes. The high specific capacitance of 164Fg−1 is obtained from cyclic voltammetry measurement at a scan rate of 10mVs−1. When the current densities are set as 3 and 6Ag−1, the specific capacitance values still reach 139 and 100Fg−1, respectively. The high capacitance is attributed to nitrogen atoms in oxidation product of p-phenylene diamine (OPPD) adsorbed on the surface of the graphene nanosheets. The comparable results suggest potential application to electrochemical capacitors based on the graphene nanosheets.