The homogeneous electrocatalytic reduction of 1,2-dihaloethanes by anions of larger fullerenes, C-76, C-78, and C-84, is presented, and structure-reactivity correlations are derived by including our data reported earlier for the C-60 and C-70 electrocatalytic process. Cyclic voltammetry measurements indicate that dianions of C76 and C-78, as well as trianions of C-76, C-78. and C-84, electrochemically generated in 0.1 M (TBA)PF6, in benzonitrile, catalyze dehalogenation of 1,2-dihaloethanes. Values of the second-order rate constant, k, for the electrocatalytic dehalogenation of 1,2-dihaloethanes by the fullerene anions were determined by using the rotating-disk electrode voltammetry under pseudo-first-order conditions with respect to the 1,2-dihaloethanes. For each fullerene anion, k increases in the order: Cl < Br < I for the investigated 1,2-dihaloethanes. Also, log k linearly increases in the order: C-84 < C-78 < C-76 < C-70 < C-60, as a function of respective redox potentials of the fullerene, for each 1-,2-dihaloethane. Unlike the C-60(n-) electrocatalysis, reported by us earlier to be accompanied by chemical reaction between C-60(n-) and certain alpha,omega-diiodoalkanes yielding alkyl adducts of C-60, no reaction between the anions of larger fullerenes and 1,2-dihaloethanes was observed within the voltammetric time scale. Because of the high stability with respect to adduct formation and more positive potentials of the electrocatalyses, the larger fullerenes may be more useful than C60 as catalysts, even though the corresponding catalytic rate constants are smaller.