To improve the processing efficiency and the surface properties of C61900 Cu alloy, a gradient Cu-Ti film with a Ti/Cu atom ratio of 7:1, 7:4, and 1:2 was pre-fabricated by the unbalanced magnetron sputtering process and then nitrided by thermos plasma nitriding. The phase structure, elemental composition, and morphology of the modified surface were characterized, and the mechanical properties, including the wear resistance and adhesion properties, were examined. Combining calculation by the first principle method with thermodynamic analysis, the microstructural formation and phase composition of the Cu-Ti-N system were investigated to reveal the mechanism of improved wear resistance, which indicated the possible formation of various Cu-Ti intermetallics and Ti-N compounds. The Al in the C61900 Cu substrate also participated in the generation of the AlCu2Ti compound, which is a ductile phase with good hardness and elastic modulus. Based on the results of a mechanical properties test, it was concluded that an optimized layer structure for the multi-phase coating should include Ti-N compounds as the surface layer and Cu-Ti intermetallics as the intermediate layer.