A new trinuclear iron(II) complex involving two isocyanoferrocene ligands axially coordinated to iron(II) phthalocyanine, (FcNC)(2)FePc [Fc = ferrocenyl; Pc = phthalocyaninato(2-) anion], was isolated and characterized using a variety of spectroscopic methods as well as single-crystal X-ray diffraction. The redox behavior of the above molecular wire was investigated through electrochemical, spectroelectrochemical, and chemical oxidation approaches and compared to that of the bis(tert-butylisocyano)iron(II) phthalocyanine reference compound, (t-BuNC)(2)FePc. For both complexes, the first oxidation involves the phthalocyanine ligand and results in the formation of a red phthalocyanine cation-radical-centered [(RNC)(2)FePc](+) species, as evidenced by their UV-vis and electron paramagnetic resonance spectra. Despite the similar to 11.5 angstrom distance between the isocyanoferrocene iron centers, the second and third oxidation potentials for (FcNC)(2)FePc are separated by similar to 80 mV, which is indicative of a weak long-range metal-metal coupling in this system. Spectroscopic signatures of the mixed-valence [(FcNC)(2)FePc](2)(+) dication were obtained using spectroelectrochemical and chemical oxidation approaches. These experimentally assessed characteristics were also correlated with the electronic structure, redox properties, and spectroscopic signatures predicted by density functional theory (DFT) and time-dependent DFT analyses.