A new chemical synthesis method to obtain a high yield of nickel nanoparticles (Ni-NPs). The morphology and crystallinity of the synthesized Ni-NPs depended on solvent and surfactant. Ethanol was found to be the best solvent in terms of complete reduction of the precursor. Surfactants impeded the agglomeration and surface oxidation of Ni-NPs. Ni-NPs were used as catalysts to synthesize of Ni/NiO-multi-layer graphene using CVD.