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The synthesis, structure, and reactivity of some organometallic-fused heterocycles were studied. This work was divided into three parts: first, thiapentalenyl tricarbonyl manganese complexes [Mn(CO)3{η5-SC7H3-1,3-(R)2}] were synthesized employing thiation on diacyl precursors; second, attempts to form the 5,5-fused ring pyrrole analogs to the thiapentalenyl complexes led to the formation of various amine and imine ligands and manganese complexes, but not the desired ring-closed pyrroles; third, reductive amination on a ferrocenyl monoaldehyde substrate led to the formation of di(N-(ferrocenylmethyl))-N-methylamine and its cyanoborane and cyanoborohydride analogs. Isolation of the desired thiapentalenyl manganese complexes was accomplished by first forming 1,2-diacylcyclopentadienes (fulvenes), converting to the corresponding thallium salts [Tl{1,2-C5H3(COR)2}] employing thallium ethoxide, transmetallating with [Mn(CO)5Br], and ring closing using either P4S1