Photoinduced charge separation of fullerodendrimers with carboxylates at terminal sites (C60 approximately COO-) has been found in aqueous media. Time-resolved transient absorption and fluorescence measurements of the fullerodendrimers demonstrated that charge separation takes place from the terminal carboxylate anion to the central excited singlet state of C60, generating C60*- approximately COO* with high quantum efficiency in aqueous solution. In the presence of viologen dication and a sacrificial donor, the persistent viologen radical cation was generated.