The amorphous alloy application is limited because of its brittleness property. Based on the grain structural characteristics of nanocrystal alloys, the mechanical behavior of the amorphous/nanocrystal Ni-Mo23.56 alloy is investigated in this text. The microstructure of the deposit and the crack propagation were discussed using scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The experimental results show that amorphous/nanocrystal Ni-Mo23.56 alloy has a higher microhardness, a strong binding force between a certain thickness coating with the substrate. The tensile stress-strain pattern shows a certain degree of plastic deformation behavior in the coating and tensile fracture surface of radial vein structure, in line with the free volume fracture model.