Multicomponent Ti-Cr-Al-N coatings with crystallites from 10 to 100 nm in size are obtained by vacuum-arc ion-plasma deposition. The dependence of the changes in the structure and phase composition of coatings on the parameters of deposition is established. An increase in the electric displacement potential (U b) applied to the substrate leads to an occurrence of CrN in the coating in addition to complex nitride (Ti, Cr, Al)N and the TiCrN2 phase. When the arc current at the chromium cathode (I Cr = 130 A) and U b are maximal, the second nitride Cr2N is produced. The emergence of chromium nitride phases is accompanied by a decrease in the size of crystallites in the coating structure. The values of both the strength of coatings (up to 32 GPa) and the elastic modulus (up to 700 MPa) are determined by the crystallite size and microstrains; the latter occur owing to chemical inhomogeneity and may reach up to 0.74%. The adhesion strength of the coatings is characterized by values on the order of 90 N. Cutting hard-alloy tools with these coatings exhibit high coefficients of resistance during uninterrupted and interrupted cutting of steel 38XHMA, which reach 5.1 and 5.7, respectively.