Growth of solid tribofilms between moving partssubstantially reduces friction and wear, and this is true especiallyfor boundary-lubricated sliding contacts. However, efficacy of thetribofilms relies upon antiwear additives in formulated oil, typicallyzinc dialkyldithiophosphate, that usually gives rise to adverseenvironmental impacts. It is desirable to reduce the use ofenvironmentally harmful additives by designing materials ofmoving parts so that they function properly with base oillubrication. Herein, CoAl layered double hydroxide (LDH)nanoplatelets were synthesized via a one-step hydrothermalapproach. When being lubricated with polyalphaolefin base oil(PAO 4), epoxy nanocomposites reinforced with low-loading LDHexhibit excellent tribological performance. In comparison to neat epoxy, wear of the nanocomposite is reduced by an order ofmagnitude and friction is decreased by 32%. Our work provides direct evidence that LDH released onto a friction interface facilitatestribofilm growth compensating for lubrication insufficiency of the oilfilm. This work paves a route for minimizing the dependencyon harmful antiwear additives by optimizing tribomaterials.