Although diamond‐like carbon (DLC) films are known for their low friction and wear properties in atmospheric environments, they commonly experience failure in vacuum environments. On the other hand, MoS 2 exhibits a low friction coefficient under vacuum conditions, but its columnar structure limits its load‐bearing capacity and results in high wear rates. In this study, we prepared MoS 2 /DLC multilayer films using a high‐power impulse magnetron sputtering (HIPIMS) technique and examined the composition, bonding structure, mechanical properties, and frictional wear of the resulting films. The study findings revealed that the multilayer film exhibits a significantly low coefficient of friction (0.04), particularly in vacuum conditions (5 × 10 −3 Pa). Remarkably, compared to the pure MoS 2 film, the wear rate of the multilayer film is reduced by two orders of magnitude, wear rate as low as 3.6 × 10 −9 mm 3 /Nm. Additionally, the DLC component enhances the hardness and reduces the wear rate of the multilayer film. Furthermore, the use of nanometer thickness (17 nm) allows for the incorporation of more MoS 2 and DLC layers, which promotes the formation of graphene bands and further reduces the friction coefficient and wear rate. Our findings open new avenues for the application of MoS 2 and DLC in vacuum environments.