This study examines the effects of lignite fly ash as a filler on the tribological and mechanical performance of a Calotropis gigantea fiber–epoxy composite. The investigation results show that the Calotropis gigantea fiber/epoxy composite with 2 wt.% lignite fly ash nanofiller added had better tensile strength, interlaminar shear, impact strength, and flexural strength than the control sample by 29.83%, 58.17%, 69.16%, and 11.41%, respectively. The manufactured composite samples were subjected to tribological tests, such as the friction coefficient and specific wear rate under dry sliding conditions with various process variables, such as sliding speed (1–3 m/s), functional load (10, 20, and 30 N), and sliding distance (1000 m). The results show that adding 3 wt.% nanofiller lignite fly ash to the Calotropis gigantea fiber/epoxy composites greatly improves the specific wear rate and friction coefficient. Additionally, the performance of the Calotropis gigantea fiber/epoxy composites in absorbing moisture was enhanced by the inclusion of the nanofiller lignite fly ash 2 wt.%. Likewise, the composite sample developed with the ideal nanofiller lignite fly ash with Calotropis gigantea fiber may be used for sustainable brake materials owing to its superior mechanical and tribological qualities.