A two-step treatment, oxidation in air followed by reduction in hydrogen, was carried out to modify the smooth Ni3Al foil surface into Ni particles supported on the oxide structure. The surface structure significantly changed depending on the oxidation temperature. A layer of granular NiO formed on the outer surface and inner oxide zone (IOZ) over Ni3Al foil surface after oxidation at 973 K. The IOZ was a mixture of Al and Ni oxides. In contrast, a large amount of faceted NiO particles formed on the outer surface after oxidation at 1173 K. Beneath the NiO particles, NiAl2O4 thin layer formed on IOZ over Ni3Al foil surface. And then, these NiO was selectively reduced to Ni after reduction treatment, constituting an oxide supported Ni particles structure. These results suggest that it is possible to modify the surface structure of Ni3Al foils simply by oxidation-reduction treatment.