Ultra-low friction coefficients and prolonged atmospheric lifetime for hydrogenated amorphous carbon (denoted a-C:H) films remain a significant challenge in the research of present. In this work, a reactive magnetron sputtering deposition facility was employed to fabricate sp 2-rich a-C:H films via metal-induced self-assembly route in the presence of Ti catalyst. The microstructure and composition of the as-prepared composite films exhibited significant variability with Ti content, particularly characterized by an abundance of sp 2 nanocrystallites embedded within amorphous carbon matrix. Moreover, the tribological behaviors and mechanical properties of Ti/a-C:H composite films were explored. The results showed that the formation of sp 2-C nanocrystallites strengthened the Ti/a-C:H composite films from 9.8 GPa to 11.2 GPa and improved the adhesion from 19.5 N to 29.7 N. Meanwhile, the as-deposited films with sp 2 nanocrystallites structure presented extremely low friction coefficient. And the characterizations of wear tracks and rubbing pairs revealed that plentiful sp 2-C nanocrystallites that originated from Ti-promoting effect aggregate at sliding surfaces between the film and the rubbing pair, resulting in outstanding tribological behavior. Especially, the film deposited at 40 % methane flow ratio exhibited superior wear lifetime ~1400 m with 0.083 friction coefficient, which showed promising potential in the industrial application as the solid lubrication film.