Vibrational frequencies of fullerene C70 and fulleride C706- have been calculated with density functionaltheory at the B3LYP/6-31G* level. Raman activities are calculated using polarizability derivatives estimatedby Hartree−Fock approximation. Good agreement with experiment is achieved when the calculated vibrationalfrequencies are uniformly scaled by a factor of 0.98 for C70. Strong Raman peaks of C70 are assigned on thebasis of both frequency and intensity information. Assignment for the weak Raman peaks is proposed. Thecalculated vibrational frequencies and intensities of C706- are presented. The intensity changes of IR andRaman peaks on going from C70 to C706- are also addressed.