Three-dimensional ordered macroporous Ni films, known as Ni inverse opals, are fabricated via a template approach in which polystyrene (PS) microspheres (820 nm in diameter) are assembled in closely-packed colloidal crystals via a vertical electrophoresis process, followed by electroplating of Ni into the interstitial voids within the colloidal crystals and the selective removal of PS microspheres. To improve its mechanical strength, a conformal Ni-Co layer (45 ∼ 64 nm) is electrodeposited on the skeletons of the Ni inverse opals by cyclic voltammetry. After coating, from nano-indentation tests, the hardness and reduced elastic modulus are enhanced considerably (172 ∼ 220% for hardness; 72 ∼ 79% for reduced elastic modulus), as compared to those of pristine inverse opals. After an annealing treatment for the interdiffusion of Ni and Co, the sample reveals an even stronger hardness. X-ray diffraction patterns indicate that the finite thickness of the inverse opals skeletons induces preferential growth of the (111) plane. In short, a combined effect of solid solution alloying, thickening of inverse opals skeletons for greater load bearing, and a predominant (111) plane is responsible for the improved mechanical strength of the Ni inverse opals.