Surface and interfacial engineering of nanomaterials is essential for improving dispersion stability in liquids. In this study, we report that oleic acid (OA)-and stearic acid (SA)functionalized layered double hydroxide (LDH) nanosheets as lubricant additives can achieve high dispersion and reduce friction and wear. LDH is a typical layered structure, and OA and SA are long-chain organic molecules that are not only compatible with base oils but also act as friction-reducing agents. The OA and SA molecules were branched onto ZnMgAl LDH nanosheets using dehydration condensation between the exposed OH groups on the surface of LDH and the COOH groups on the OA and SA molecules. Compared with that of the pristine ZnMgAl LDH, the dispersion of OA-ZnMgAl LDH and SA-ZnMgAl LDH was significantly improved. The surface-modified LDH exhibited superior tribological properties and great stability due to the synergistic lubrication effect between OA, SA, and LDH. Even at an ultralow concentration (0.15 wt %), the coefficient of friction and wear volume were reduced by ∼65 and ∼99%, respectively, compared to those of the base oil. Due to the green and simple synthesis method and excellent tribological properties, surface-functionalized LDH has enormous possibilities for future industrial applications.