The compounds cis-Mo-2(DAniF)(2)(L)(2) have been prepared, where DAniF = (N,N'-p-dianisyl formamidinate and L = thienyl-2-carboxylate (Th), 2,2'-bithienyl-5-carboxylate (BTh), and 2,2':5',5 ''-terthienyl-5-carboxylate (TTh). The compounds have been characterized by proton nuclear magnetic resonance (H-1 NMR), ultraviolet-visible (UV-vis) absorption and emission, differential pulse voltammetry, and time-resolved transient absorption and infrared (IR) spectroscopy. An X-ray crystal structure was obtained for the thienyl complex. The related salt [(Bu4N)-Bu-n](2)[Mo-2(DAniF)(2)(TTh-CO2)(2)], where TTh-CO2 = 2,2':6',2 ''-terthienyl-5,5 ''-dicarboxylate, has also been prepared and employed in the attachment of the complex to TiO2 nanopartides. The latter have been characterized by ground-state Fourier transform infrared spectroscopy (FTIR) and femtosecond time-resolved IR spectroscopy. The time-resolved data provide evidence for sub-picosecond charge injection from the Mo-2 center to the semiconducting oxide particle.