As a high-temperature structural material, Ni3Al matrix composites are often used to manufacture basic mechanical components that need to be used in high-temperature conditions. To meet the increasing demand for metal matrix composites with an excellent tribological performance over a wide temperature range, Ni3Al matrix self-lubricating composites containing Sn-Ag-Cu and Ti3SiC2 (NST) were synthesized via laser-melting deposition. Dry sliding friction tests of NST against Si3N4 ball were undertaken from 20 to 800 °C to investigate the tribological behavior and wear-triggered self-healing properties. The results show that the tribological behaviors of NST are strongly dependent on the testing temperature and self-healing properties. At low and moderate temperatures from 20 to 400 °C, as the Sn-Ag-Cu flows into the cracks and is oxidized during sliding friction, while the cracks on the worn surface are filled with oxides consisting mainly of Al2O3, SnO2 and CuO. At higher temperatures of 600 and 800 °C, the cracks are filled by the principal oxides of Al2O3, TiO2 and SiO2 due to the partial decomposition and oxidation of Ti3SiC2. Compared with other testing temperatures, the recovery ratio relative to the Ni3Al base alloy of the cracks on the worn surface of NST is the highest at 400 °C, which is about 76.4%. The synergistic action mechanisms of Sn-Ag-Cu and Ti3SiC2 on the crack self-healing from 20 to 800 °C play a significant role in forming a stable solid lubricating film, improving the anti-friction and wear resistance of NST. The results provide a solution allowing for metal matrix composites to achieve excellent lubrication stability over a wide temperature range by virtue of the crack self-healing properties.