In this study, aluminum alloys were subjected to nitriding at 823 K for 0–18.0 ks using alumina and magnesium powders for improving their radiation performance. After nitriding, aluminum nitride films were formed on the aluminum substrate. The thickness of the formed films varied from 1.5 to 11 μm, and the color of the film surface was dark brown or black. The thickness of the aluminum nitride film increased with an increase in the treatment time. X-ray diffraction and electron probe microanalysis results showed that the film was composed of aluminum nitride, alumina, aluminum, and magnesium. Further, the film showed good adhesion at 0 ks.