Abstract Carbon nanotube (CNT) buckypaper (BP) is a kind of non-woven nano-fiber film with excellent mechanical and electrical properties. Herein, we applied it to enhance the tribological performance of epoxy resin. A relatively big BP film with a diameter up to 285 mm was obtained through a solution filtration method. The CNTs were surface-modified by ozone in order to improve their interfacial adhesion with the matrix. It was found that the CNTs were well impregnated by the epoxy resin and the interfacial adhesion was fairly good, especially for the modified ones. The wear tests were performed using a ball-on-disc (“steel-on-polymer”) configuration under dry sliding condition. Depending on the conditions of the wear tests, the frictional coefficient can be reduced from 0.71 of the neat resin down to 0.32 of ozone-modified BP/epoxy composite and the wear resistance can be improved by more than 4 times. The SEM morphologies and Raman spectra of worn surfaces for the samples were given to explain the possible wear micro-mechanisms. The BP/epoxy composites, even after subjected to harsh wear, still retained high electrical conductivity due to the robust CNTs network.