Reduced fullerenes and fullerene derivatives exhibit intense absorptions in the vis-near-IR (vis-NIR) region. The absorptions are sensitive toward the addition pattern, number of addends, and oxidation state of the fullerene species and are used as an important benchmark for identifying anionic fullerene species. Similar absorptions are also shown for the reduced singly bonded C-60 species, which are electronically different from reduced fullerene derivatives. However, much less work has been carried out on the vis-NIR spectroscopic study of the anionic singly bonded C-60 species, likely due to the difficulty in controlled production of these species. Herein, we report the vis-NIR spectroscopic study of the mono- and dianions of the singly bonded C-60 species (RC60-, R-C60-, and RC602-center dot), which are selectively generated by controlled-potential bulk electrolysis (CPE) of the singly bonded C60 dimer and C-60 oxazolino heterocycles. Time-dependent density functional theory (TD-DFT) calculations were performed to rationalize the experimental results.