With increasingly harsh working environments for mechanical systems and the rapid development of various high-tech industries, requirements for the stable operation of mechanical systems are increasing in a wide temperature range. Mo and S co-doped CrN coatings with different MoS2 contents were prepared via unbalanced magnetron sputtering to provide better friction properties to the coatings at high temperatures. Scanning electron microscopy and nanoindentation were adopted to analyze the microstructure and mechanical performance. The mechanical performance of the coatings was enhanced by increasing the MoS2 content, however, excessive MoS2 reduced the mechanical properties of the coatings. Besides, the adhesion of the coating first increased to 33.08N and then decreased rapidly to 7.24N. In addition, the residual stress of the coating first decreased and then increased upon increasing the MoS2 content. The high-temperature tribological behavior of the coatings was measured from room temperature (25 ℃) to 600 ℃. The friction and wear coefficient of CrN/MoS2-0.6A coating decreased by 12.9% (0.67) compared with other coatings at room temperature and relatively good comprehensive properties at high temperature. This study provides a feasible design for engineering applications and lays the foundations for the preparation of coatings with superior high-temperature friction properties.