The addition of nanoparticles to water-based lubricants is a commonly used method to improve lubrication, but to the best of our knowledge few studies have been reported to investigate the lubrication property of surface-modified nanodiamonds (ND) with polyzwitterionic brushes. In this study, a bioinspired copolymer containing dopamine and 2-methacryloyloxyethyl phosphorylcholine (MPC) was synthesized (DMA-MPC) and then spontaneously grafted onto the ND surface (ND-MPC) through simple stirring in order to enhance lubrication. The characterization of transmission electron microscopy, Fourier transform infrared spectroscopy, and thermogravimetric analysis indicated that the DMA-MPC was successfully modified on the ND surface. Furthermore, a series of tribological experiment were performed on a universal materials tester using glycerol, glycerol + ND, and glycerol + ND-MPC as the lubricants. It was found that the addition of ND to the lubricant (i.e., glycerol + ND and glycerol + ND-MPC) significantly reduced wear with a smaller wear scar and wear track on the tribopairs, and the coefficient of friction further decreased by about 40% when using glycerol + ND-MPC as the lubricant, which could be attributed to the hydration lubrication of the polyzwitterionic brushes modified on the ND surface and the rolling effect of nanoparticles. In conclusion, in this study a universal and versatile surface modification method was proposed on the basis of the synthesis of bioinspired copolymer DMA-MPC, which remarkably enhanced the lubrication property of ND nanoparticles when added to water-based lubricants.