In this study, MoS2 solid lubricant films were supported with crystalline TiNi films for the first time in the literature to produce functional solid lubricant coatings. The structural, mechanical, and tribological properties of the produced coatings were investigated. The functional coatings were deposited on 52100 bearing steels by the Closed Field Unbalanced Magnetron Sputtering System (CFUBMS). SEM, XRD, EDS, and DSC analyses were used to obtain structural properties. A pin-on-disc Wear Test at atmospheric and high-temperature conditions was carried out to analyse the tribological behaviors of the coatings. The results showed that the TiNi/MoS2 functional coating had great tribological properties. S/Mo ratio and thickness and hardness values of the coatings directly affected tribological properties. The friction coefficients decreased as the S/Mo ratio of the coatings approached 1.5. Tribological properties generally increased as the hardness and thickness of the coatings increased. CoF values lower than 0.1 were obtained at atmospheric and high-temperature wear tests.