Ni-Mo alloys have been studied as a prospected cathode for its higher hydrogen evolution reaction properties than other binary compounds. X-ray diffraction (XRD) analysis and scanning electron microscopy (SEM) microstructures show that the amorphous/nanocrystal Ni-Mo deposits were deposited. The Ni-Mo deposits cathode are electrolyzed in 25°C, 7 mol/L NaOH electrolytic solution. And when η100, the amorphous/nanocrystal Ni-Mo alloy with a lower hydrogen evolution overpotential, a higher exchange current density, and a better electrolytic stability is lower than amorphous Ni-Mo deposits. This is due to the amorphous content combined with nanocrystalline structure, lager contact surface and binding energy of Ni-Mo structure.