Pure MoS2 films exhibit disadvantages such as low densities, poor mechanical properties, and weak wear resistance under atmospheric environments. For this reason, Ti was chosen as the doping element in this work. Mo-S-Ti composite films with different Ti contents were deposited using the magnetron sputtering system, and the effects of Ti content on the chemical composition, mechanical and tribological properties of these films were analyzed by numerous characterization methods to determine the doping content of Ti elements. The results show that the tribological performance of Mo-S-Ti composite film under atmospheric environments reaches the best when the Ti content is 13.48 at%. In addition, the present work also found that longitudinal load and reciprocating frequency have a significant effect on the tribological properties of this film. It is easier to form high quality transfer film on GCr15 balls under higher longitudinal load and lower reciprocating frequency, thus transforming the friction between film and GCr15 ball into the friction between film and transfer film, resulting in excellent tribological performance.