Mechanical, physical and tribological properties of layer-gradient multi-component coatings based on the Mo–S–Ti–C composition are investigated. The coatings are formed by combining the magnetron sputtering and the hybrid magnetron and vacuum arc deposition assisted by a gas plasma generator. A correlation is established between the physic mechanical and tribological properties of the resulting coatings, which allows identifying their potential applications. The physical principles of the combined technologies of lowtemperature ion-plasma deposition of tribological Mo–S–Ti–C coatings onto hardened steel machine parts are developed.