Abstract: | The title compounds with terminal N‐heterocyclic carbenes, namely octacarbonyl(imidazolidinylidene‐κC2)di‐μ3‐sulfido‐triiron(II)(2 Fe—Fe), Fe3(C3H6N2)(μ3‐S)2(CO)8], (I), and octacarbonyl(1‐methylimidazo1,5‐a]pyridin‐3‐ylidene‐κC3)di‐μ3‐sulfido‐triiron(II)(2 Fe—Fe), Fe3(C8H8N2)(μ3‐S)2(CO)8], (II), have been synthesized. Each compound contains two Fe—Fe bonds and two S atoms above and below a triiron triangle. One of the eight carbonyl ligands deviates significantly from linearity. In (I), dimers generated by an N—H...S hydrogen bond are linked into 001] double chains by a second N—H...S hydrogen bond. These chains are packed by a C—H...O hydrogen bond to yield 101] sheets. In (II), dimers generated by an N—H...S hydrogen bond are linked by C—H...O hydrogen bonds to form 111] double chains. |