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Lanthanide complexes are known to be one of the most valuable catalysts, due to their high activity and/or excellent controllability.[1] The remarkable effect of alkali metal on catalytic reactivity of samarium-alkali metal clusters is systematically studied.Three samarium clusters--Sm2Na8(OCH2CH2NMe2)(OH)2(1),[2] Sm4K20(OCH2CH2NMe2)26(OH)6(2), Sm2K12Na4(OCH2 CH2NMe2)8(OH)4(3) are synthesized in high yield.