The electronic transitions of C60+ and C60- isolated in 5 K neon matrices were detected with well-resolved vibrational structure after NeI irradiation of C60 during deposition. On the basis of a C60+ spectrum obtained by growing a matrix with a mass-selected C60+ ion beam, overlapping peaks in the electronic spectra were assigned to either C60+ or C60-. The vibrational frequencies 1406 and 1332 cm-1 for C60+, and 1386 and 1202 cm-1 for C60-, were identified in a neon matrix from the infrared spectrum. C60- was also detected after codepositing Na and K with C60, without irradiation. Relevance of the data to interstellar observations is discussed.