In this study, we used a four-ball friction and wear testing machine to test the tribological properties of [HPy]BF4 ionic liquids (ILs), low-layer graphene (G), and IL and G compounds (IL/G) as lubricant additives at variousconcentrations, loads, and speeds. The morphology of the wear scar was characterized by a white-light interferometer and a scanning electron microscope (SEM). The results showed that the optimal concentrations of IL and G were 0.10[Formula: see text]wt.% and 0.05[Formula: see text]wt.%, respectively. When the IL concentration was 0.10[Formula: see text]wt.%, the friction coefficient and the wear scar diameter (WSD) reduced by approximately 18% and 8%, respectively, compared to the base oil. When the concentration of G was 0.05[Formula: see text]wt.%, the friction coefficient and WSD reduced by approximately 23% and 12%, respectively, compared to the base oil. After adding the optimal concentration of the IL/G composite additive under the same test conditions, the average friction coefficient of the steel ball reduced by approximately 30%, and the average WSD reduced by approximately 18%. IL/G nanoadditives could be easily attached to the pit area on the friction surface of the steel ball, which made the contact surface of the friction pair smoother and the area of the oil film bearing the load larger, compared to those using the base oil. These two combined phenomena promoted synergistic antifriction and antiwear effects, which significantly improved the frictional performance of the base oil.