The first spectroscopic characterization of the dimeric dicationic fullerene complex [(C-70)(2)](2+)(Ti3Cl13)(2)(-) is reported and supported by DFT calculations. The IR spectrum of the dimer is interpreted in terms of the normal modes of the pristine C-70, and the effects of charging C-70 and the intercage bond formation between C-70 units on the IR spectrum are discussed. Analysis of the vibrational spectrum of the anion, Ti3Cl13-, is also provided. NIR absorption and fluorescence spectra of the complex are studied, and the dimer is shown to have a small HOMO-LUMO gap of 0.8 eV. The electronic structure of [(C-70)(2)](2+) is studied with the use of DFT and compared to that of the other single-bonded fullerene dimers, including [(C-70)(2)](2-), (C69N)(2), and [(C-60)(2)](2-). Characteristic features in the vibrational spectra and electronic structure of all single-bonded fullerene dimers are revealed.