Ni/ZrO 2 and Ni/(Zr 0.9 Sm 0.1 ) 0.95 catalysts were prepared by wet impregnation, and their catalytic activities for methanation of carbon dioxide were compared with the highly active catalysts prepared from amorphous nickel-zirconiumsamarium alloys. The Ni(Zr 0.9 Sm 0.1 )O 1.95 catalyst showed higher activity for methanation of carbon dioxide than the samarium-free Ni/ZrO 2 catalyst with the same nickel content. The higher activity of the samarium-containing catalyst is associated with the formation of the (Zr-Sm)O x oxide with a tetragonal ZrO 2 structure, similar to the Ni/(Zr-Sm)O x catalysts prepared from the amorphous nickel-zirconium-samarium alloys. An increase in the nickel content from 30 to 60 mol% in cationic percentage results in a decrease in the activity, mainly because of a decrease in the surface area of the catalysts, although the activity of the catalysts prepared from amorphous nickel-zirconium-samarium alloys increases with the nickel content. Further, it was found that the activities of the Ni/(ZrSm)O x catalysts prepared from the amorphous nickel-zirconium-samarium alloys are higher than those prepared by wet impregnation. Uniform dispersion of nickel in the catalysts prepared from amorphous single-phase alloys should be one of the reasons for the extremely high activity of the catalysts.