Toluene solutions of C-60 react upon UV irradiation with Fe2S2(CO)(6) to give C-60[S2Fe2(CO)(6)](n) where n = 1-6. C-60[S2Fe2(CO)(6)](n) where n = 1-3 have been isolated and characterized. Crystallographic studies of C60S2Fe2-(CO)(6) show that the S-S bond of the Fe-2 reagent is cleaved to give a dithiolate with idealized C-2v symmetry. The addition occurred at a 6,6 fusion, and the metrical details show that the Fe-2 portion of the molecule resembles C2H4S2Fe2(CO)(6). IR spectroscopic measurements indicate that the Fe-2(CO)(6) subunits in the multiple-addition species (n > 1) interact only weakly. UV-vis spectra of the adducts show a shift to shorter wavelength with addition of each S2Fe2(CO)(6) unit. Photoaddition of the phosphine complex Fe2S2(CO)(5)(PPh(3)) to C-60 gave C-60-[S2Fe2(CO)(5)(PPh(3))](n), where n = 1-3. P-31{H-1} NMR studies show that the double adduct consists of multiple isomers. Photoaddition of Fe2S2(CO)(6) to C-70 gave a series of adducts C-70[S2Fe2(CO)(6)](n) where n = 1-4. HPLC analyses show one, four, and three isomers for the adducts, respectively.