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In this study, a compound filler consisting of zinc sulfide (ZnS) nanoparticles and reduced graphene oxide (RGO) was synthesized using the hydrothermal method and utilized to enhance the tribological properties of the polyimide (PI) film. The ZnS@RGO/PI composites displayed the lowest wear rate of 3.89 × 10
−8
mm
3
N
−1
m
−1
at a load of 200 N, which were significantly lower than that of both pure PI and RGO/PI films. Furthermore, the microstructure and chemical composition of the compound were characterized and analyzed, revealing that the ZnS nanoparticles were effectively attached to the surface of RGO through the chemical bonding between them. Finally, finite element analysis shows that the chemical bonding between ZnS and RGO have the effect to stop the crack expanding under pressure, and a wear mechanism is also given to demonstrate this ‘Ball-on-plane’ compound’s enhancement to the tribological properties.