The 1 : 2 reaction of the imidazole‐based dithiolate (
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Abstract 2 ) with GeCl2 • dioxane in THF/TMEDA gives3 , a TMEDA‐complexed dithiolene‐based germylene. Compound3 is converted to monothiolate‐complexed (5 ) and N‐heterocyclic carbene‐complexed (7 ) germanium(II) dithiolene complexes via Lewis base ligand exchange. A bis‐dithiolene‐based germylene (8 ), involving a 3c–4e S‐Ge‐S bond, has also been synthesized through controlled hydrolysis of7 . The bonding nature of3 ,5 , and8 was investigated by both experimental and theoretical methods.