We report here experimental evidence for the formation in the solid state of a new binuclear Fe-2(III) (mu-OMe)(2)(HL)(4) complex (H2L is 2-salicyloylhydrazono-1,3-dithiolane). The isostructural Mn-2(III)(mu-OMe)(2)(HL)(4) complex has provided the strongest ferromagnetic interaction value (J approximate to 20 cm(-1)) between Mn-III ions to date. The new iron binuclear compound presented in this study shows antiferromagnetic intramolecular coupling, which agrees with the theoretical study that we previously proposed. During our synthetic work, we also observed an unexpected spontaneous reduction of the new Fe-III(HL)(2)Cl,S complex to the new Fe-II(H2L)(2)Cl-2 high-spin mononuclear complex. This process has been checked by cyclo-voltammetry as well as pseudosteady voltammetry.