We prepare Cu/Ni bilayer films by depositing the incident atoms on Cu substrates with various surface orientations and under different temperatures and investigate interfacial structure, surface roughness, radial distribution function and hardness of the films. We find that the incident atoms can penetrate (001) substrate more easily than other surfaces, resulting in a transitional layer consisting of two kinds of atoms. Stacking faults are generated in the bilayer films deposited on the (111) substrate, which can reduce misfit strain and thus account for the layer growth mode of the films. The surface roughness decreases with the increase in deposition temperature. Moreover, we also find that a certain degree of roughness benefits the formation of coherent interface due to the tilted-layer epitaxial growth. The hardness differs for the films deposited at different temperatures.