In this work, we report the synthesis and a study on the degree of electronic delocalization in the asymmetric mixed valence complexes [Cp*Fe(C8H6)Fe(C8H7)](+), 3a(+), and [Cp*Co(C8H6)Fe(C6H7)](+), 3b(+), (Cp* = C5Me5, C8H6 = pentalenyde, C8H7 = hydropentalenyde, and BAr'(4) = ((3,5(CF3)(2)C6H3)(4)B (-))). Electrochemical methods, Fe-57 Mossbauer spectroscopy, electronic spectroscopy, and electron paramagnetic resonance were used for this purpose. Although the anti conformation of the complexes precludes any metal-metal interaction, all the techniques employed show that 3a(+) is a electronic delocalized system, while 3b(+) behaves as two individual metallic centers with localized electron density.