Reaction of [fc(NH2)(2)]RuCl2(PPh3)(2) (fc = 1,1'-ferrocenylene) with 2 equiv of (KOBu)-Bu-t led to the formation of a diamido ruthenium complex, [fc(NH)(2)]Ru(PPh3)(2), whose solid-state molecular structure revealed a short Fe-Ru distance. A metal-to-metal charge transfer band was observed in the electronic absorption spectrum of [fc(NH)(2)]Ru(PPh3)(2). The Fe-Ru interaction was characterized by resonance Raman spectroscopy for the first time and also by H-1 NMR, UV-vis, NIR, Mossbauer spectroscopy, and X-ray crystallography. Density functional theory (DFT) calculations including natural bond order analysis, Bader's atom in molecules method, and time dependent DFT (TDDFT) provided further support that the iron-ruthenium bond is a weak donor-acceptor interaction with iron acting as the Lewis base.