Diamond-like carbon (DLC) films are deposited on rubber surfaces to protect the rubber components, and surface pretreatment of the rubber substrates prior to the film deposition can improve the adhesion between the DLC films and the rubber. Thus, the principal purpose of this work concentrates on determining the effects of argon (Ar), oxygen (O2), nitrogen (N2), and hydrogen (H2) plasma pretreatments on the adhesion and friction performance of the DLC films deposited on rubber (DLC/rubber). The results indicated that the Ar plasma pretreatment promoted the formation of a compact layer on the rubber surface. By contrast, massive fillers were exposed on the rubber surface after oxygen or nitrogen plasma pretreatments. Moreover, the typical micrometer-scale patches divided by random cracks were observed on the surface of DLC/rubber, except for the sample pretreated with oxygen plasma. The adhesion of DLC/rubber was found to strengthen with the removal of weak boundary layers and the generation of free radicals on the rubber surface after plasma pretreatment. The tribo-tests revealed that DLC/rubber with O2, N2, and H2 plasma pretreatments cannot achieve optimal friction performance. Significantly, DLC/rubber with Ar plasma pretreatment exhibited a low and stable friction coefficient of 0.19 and superior wear resistance, which was correlated to the high adhesion, good load-bearing of the rubber surface, and the approximate sine function of the surface profile of the DLC film.