The electrochemical properties of covalent derivatives of the higher fullerenes C70, C76, C2v-C78, and D3-C78, bearing bis(alkoxycarbonyl)methano addends, were investigated by cyclic voltammetry (CV) and/or steady-state voltammetry (SSV). Included in this study were a series of previously prepared mono- to tetrakisadducts of C70, monoadducts of C76, and bis- and trisadducts of C2v-C78 and D3-C78. For all compounds, several (up to five) reduction steps and one or two oxidation steps were observed. The reduction steps usually required more energy than the corresponding processes in the parent fullerenes whereas the oxidation steps became facilitated with increasing degree of addition. A notable exception to this trend was the observation that two C76 monoadducts were more readily reduced than the parent fullerene and one was more difficult to oxidize. The electrochemical properties of C70 derivatives were found to closely resemble those of C60 adducts. Constitutional isomers displayed nearly identical redox...