Si doped diamond-like carbon (Si-DLC) films were deposited on nitrile-butadiene rubber (NBR), and the effects of deposition parameters on the mechanical and tribological properties of an Si-DLC top layer on NBR were investigated. Then, the sample with the best performance is selected to investigate its tribological behaviors and mechanism under different contact loads. The results show that the growth rate and the doped Si content are also decreased with increasing the CH4 flow rate. The Si atom exists in the form of Si-C bonds at low CH4 flow rate (≤40 sccm) and Si-C + Si-O-C bonds at high CH4 flow rate (≥60 sccm). Furthermore, the sp3 content increases monotonously, while the hardness and H3/E2 ratio firstly decreases and then increases. As a result, the friction and wear behaviors are in line with the change trend of the hardness. The lowest friction coefficient (~0.19) and a slight wear were achieved for the Si-DLC3 film under the relatively high load of 3 N. The tribological results indicate that the friction coefficient and wear increase monotonously with the increase of load, which is mainly attributed to the brittle fragmentation of films at a higher load, and thus a high strength and super toughness DLC films should be needed. Furthermore, the friction and wear behaviors of samples depend critically on its surface topography, and the wear is lower when the friction direction is parallel to the stripes.