The synthesis of the first homoleptic double metallocene complex of iron, Fe(2)Pn(2)* (Pn* = permethylpentalene, C8Me6) is described. The structural and electronic properties of Fe(2)Pn(2)* have been characterized by NMR and EPR spectroscopy, single crystal X-ray diffraction, magnetic measurements, cyclic voltammetry, and DFT calculations. Fe(2)Pn(2)* adopts a C-i symmetry in the solid state with a Fe-Fe distance of 2.3175(9) angstrom, slightly lower than the sum of radii in metallic iron. Magnetic measurements in solution, and of the solid phase between 60 and 300 K, indicate that Fe(2)Pn(2)* is a triplet (S = 1) paramagnet, with effective magnetic moments (mu(eff)) of 3.4 and 3.48 mu(B), respectively. DFT calculations indicate the origin of this high magnetic moment is likely to be unquenched orbital angular momentum contributions from two SOMOs which have metal d character. Cyclic voltammetry studies demonstrate that Fe(2)Pn(2)* can access four charge states (-1, 0, +1, +2).