Friction-associated energy loss and mechanical wear leading to failure is a major problem in industries. To mitigate this, the design and testing of novel lubricants is important. Here, we show the facile one-pot synthesis of ZnO/ZnO nanorods (NRs) and MoS2 films on pre-treated glass substrates via aerosol-assisted chemical vapor deposition. The bearing capacity and wear life of ZnO film/ZnO NRs/MoS2 films were improved due to the lubricant retention capabilities of the NRs. Modification of the ZnO/MoS2 nano-arrays using polydopamine (PDA) allowed the realization of robust and ultra-stable solid lubricants through the triple action of chemical chelation, layered materials, and nanotexture, especially under heavy load conditions. Compared with pristine MoS2, the adhesion and bearing strength of the composite film increased by 11 and 30 times, respectively, while the coefficient of friction and wear rate decreased by 94 and 85%, respectively. This is because the chelation between the transition metal and the groups in the interlayer PDA was fully utilized to improve the interface compatibility, which significantly improves the robustness of ZnO NRs and the adhesion of MoS2. This allowed a stable and firm mechanical lock between the substrate, lubricant films, and the steel ball. It demonstrated a convenient method to achieve the antifriction and anti-wear of solid lubricating materials by PDA interface modification for practical industrial applications.