Tribological performance of motion components is one of the key aspects that must be considered in a wide range of applications such as vehicles, aircrafts, and manufacturing equipment. This work demonstrates that further addition of only low-loading hard nanoparticles into a formulated nonasbestos organic brake material directly switches its functionality to a selflubrication material. More importantly, the newly developed nanocomposites exhibit an extremely low wear rate. Comprehensive investigations on the friction interface reveal that the great friction and wear reduction are due to the formation of a nanostructured lubricious tribofilm. Tribofilm formation is continuously fed by complex molecular species released from the bulk nanocomposites, for which nanoparticles digested within the tribofilm greatly enhance its robustness and lubricity. This work gains insight into the crucial role of the interface nanostructure and paves a route for developing extremely wear-resistant self-lubrication composites for numerous applications.