Main regularities of the formation of microstructure and properties of multilayer nanostructured CrN/MoN films with periodically changing architecture of layers were considered. Coatings were fabricated by vacuum-arc evaporation of the cathodes (Arc-PVD) in nitrogen atmosphere (p_N was 0.4, 0.09 and 0.03 Pa). CrN and γ-Mo₂N nitride phases with fcc lattices and a small volume of metastable MoN_x cubic phase were formed in the films at p_N = 0.4 Pa. The decrease of p_N to 0.09 Pa causes the formation of β-Cr₂N hexagonal phase. Preferential crystallographic orientation changes from [311] to [111] and [200] when bias voltage U_b is −20, −150 and −300 V respectively. The nanocrystallites size in coatings with bilayer thickness λ = 44 nm decreases to 5.8 nm. The microdeformation grows from 0.4 to 2.3% when U_b changes to −20 V. Coatings show high hardness of 38–42 GPa and H/E = 0.107. In a couple with results of tribological tests, coatings demonstrate strong wear resistance, which makes them appropriate and promising for industrial applications as protective ones. The effect of deposition conditions (p_N, U_b, λ) on composition, structure, hardness, toughness and wear resistance was studied to achieve superior mechanical and physical properties of coatings with long lifetime in harsh environment