CrN/Mo2N films were deposited by multi-cathodic arc ion plating on Si (100), 304 stainless steel and cemented carbide substrates with various bilayer periods (10–105nm). X-ray diffraction analysis revealed a face-centered-cubic structure of CrN and Mo2N sublayers. Rutherford backscattering spectrometry (RBS) was used to probe the elemental composition and their depth profiling. The multilayer structures exhibited characteristic oscillating RBS spectra. The nanohardness slightly increased at larger bilayer periods and the highest value of 29GPa was obtained at the bilayer period of 105nm. A correlation was realized among compressive residual stress, critical load, and nanohardness. The highest critical load Lc2 of 65–70N was found for the coatings on cemented carbide substrates with the minimal bilayer period of 12nm. The coefficients of friction and wear rates of the coatings were in the range of 0.29–0.35 and (6–8)×10−7mm3/N·m, respectively.