Chemical oxidation and reduction of the all ferrous (L-H)(2)Fe-6 in THE affords isostructural, coordinatively unsaturated clusters of the type [(L-H)(2)Fe-6](n): [(L-H)(2)Fe-6]-[BArF24] (1, n = + 1; where [BArF24](-) = tetrakis[(3,5-trifluoromethyl)phenyl]borate), [Bu4N][(L-H)(2)Fe-6] (2a, n = -1), [P][(L-H)(2)Fe-6] (2b, n = -1; where [P](+) = tributy1(1,3-dioxolan-2-ylmethyl)phosphonium), and [Bu4N](2)[(L-H)(2)Fe-6] (3, n = -2). Each member of the redox-transfer series was characterized by zero-field Fe-57 Mossbauer spectroscopy, near-infrared spectroscopy, single-crystal X-ray crystallography, and magnetometry. Redox-directed trends are observed when comparing the structural metrics within the [Fe-6] core. The metal octahedron [Fe-6] decreases marginally in volume as the molecular reduction state increases as gauged by the Fe-Fe-avg distance varying from 2.608(11) angstrom (n = +1) to 2.573(3) (n = -2). In contrast, the mean Fe-N distances and