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Surface-enhanced Raman (SER) spectra are reported for thin films of C60 and (eta 5-C9H7)Ir(CO)(eta2-C60) on gold electrodes in acetonitrile. The latter spectra display the hallmarks of vibrational symmetry lowering for C60 arising from metal coordination, involving splitting of the normally degenerate H (sub g) modes and the appearance of vibrationally forbidden bands. Only a milder selection rule relaxation is observed for SERS of uncoordinated C60. Electroreduction of both C60 and the Ir-C60 complex yielded similar frequency downshifts in the Ag pentagonal pinch mode, indicating that electron addition to the latter is fullerene localized. These spectral shifts are sensitive to the nature of the countercation.