Reaction of carbonyl compounds (methyl acetate, acetone and acetaldehyde) with ammonia at 473-523 K over LnCu/Al2O3, Ln-Fe/SiO2, Ln-Ni/SiO2 and Ln-Co/SiO2 bimetallic catalysts, prepared by reaction of Cu/Al2O3, Fe/SiO2, Ni/SiO2 and Co/SiO2 with lanthanide metals (Ln: Eu and Yb) dissolved in liquid ammonia, respectively, were studied. Since such bimetallic catalysts have functions of hydrogenation, dehydrogenation and transfer hydrogenation from ammonia, the reaction of carbonyl compounds with ammonia were extended to amination, reductive alkylation or their related reactions. The catalytic properties varied markedly with different levels of lanthanide content in the catalysts. Ln-Cu/Al2O3 was used more efficiently when subjected to the reaction of methyl acetate with ammonia. Upon introduction of lanthanide metals onto Cu/Al2O3, Eu-Cu/Al2O3 bimetallic catalysts were highly activated for the formation of acetonitrile. Since Eu-Cu/Al2O3 showed high activity for the transfer hydrogenation in which ammonia was the donor of hydrogen, the reductive amination of acetone occurred to yield isopropylamine even without direct addition of hydrogen.