Cyano-bridged mixed valence compounds have been known since 1704, but a lot of interest in the bi- and tri-nuclear species has emerged only more recently. The growing interest in these complexes reflects their promise as useful applications in electrochromism, molecular magnetism, and molecular electronics. These properties are activated by the excitation of their metal-to-metal charge transfer (MMCT) transition. We have studied aqueous solutions of the FeHEDTA/Fe(CN)64- system that form intensely colored solutions that absorb strongly in the Vis/NIR region. Typically 1:1 dimeric and 2:1 trimeric complexes are formed. We have used optical spectroscopy and electrochemistry to provide information on reorganizational parameters, electronic coupling between metal centers, molar absorptivities, equilibrium constants, and delocalization factors and have compared results obtained for the binuclear and trinuclear species to results of similar systems either previously studied in our lab or found in the literature.