The synthesis of functionalized fullerene-C 60 (C 60 ) was performed using living anionic polymerization. The metalation of the benzylic hydrogen atom on toluene or p-substituted toluene was conducted with the alkyllithium/amine system, and examined by living anionic polymerization of 1,3-cyclohexadiene. The number of carbanions bonded onto C 60 was estimated by the grafting reaction of living polymer onto C 60 . The tert-butyllithium/ N,N,N 0 ,N 0 -tetramethylethylenediamine system was an effective metalation reagent, and toluene-, p-xylene-, 4-methyltriphenylamine-functionalized C 60 s having good solubility were successfully synthesized.