By the synthesis of Cl3Ge(CH2)2CN (1) and subsequent reaction with sodium monochalcogenides, adamantane-type [(NC(CH2)2Ge)4Ch6] (Ch = S (2), Se) and noradamantane-type [(NC(CH2)2Ge)4Te5] (3) were obtained. The compounds represent the first nitrile-functionalized tetrel chalcogenide clusters and the first nitrile-functionalized clusters of the named architectures, and are thus potential precursor for novel reaction pathways to multifunctional core-shell compounds.