Reaction of the Rieske cluster model complex (Et4N)(2)[(N2CHPh)Fe2S2(S-2-o-xyl)] (N2CHPh = dianion of 2,2'-(phenylmethylene)bis(3-methylindole); S-2-o-xyl = dianion of 1,2-phenylenedimethanethiol) with nitric oxide results in disassembly of the iron-sulfur core and-formation of {Fe(NO)(2)}(9) dinitrosytiron complexes (DNICs). Isolation and characterization of these DNICs, including the new compound, (Et4N)[N2CHPh)Fe(NO)(2)], demonstrates homology between the synthetic Riekse cluster and purely thiotate-bound Fe2S2 clusters in reactions involving NO. To-model-the nitrogen-rich environment of Rieske cluster-derived dinitroysliron species, a new:type of neutral {Fe(NO)(2)}(9) DNIC was prepared containing a beta-diketiminate ligand. One-electron reduction of this compound affords the isolable {Fe(NO)(2)}(10) DNIC. These-compounds represent a rare example of structurally analogous DNIC redox partners.