Titanium and its alloys are widely used in high-end manufacturing fields. However, their low high-temperature oxidation resistance has limited their further application. Recently, laser alloying processing has attracted researchers to improve the surface properties of Ti, for which Ni coated graphite system is an excellent prospect due to its outstanding properties and metallurgical bonding between coating and substrate. In this paper, nanoscaled rare earth oxide Nd2O3 addition was added to Ni coated graphite laser alloying materials to research its influence on the microstructure and high-temperature oxidation resistance of the coating. The results proved that nano-Nd2O3 has an outstanding effect on refining coating microstructures, thus the high-temperature oxidation resistance was improved. Furthermore, with the addition of 1. 5 wt.% nano-Nd2O3, more NiO formed in the oxide film, which effectively strengthened the protective effect of the film. After 100 h of 800 °C oxidation, the oxidation weight gain per unit area of the normal coating was 14.571 mg/cm2, while that of the coating with nano-Nd2O3 addition was 6.244 mg/cm2, further proving that the addition of nano-Nd2O3 substantially improved the high-temperature oxidation properties of the coating.