Addition of the C-60 moiety, a powerful electron acceptor, to iodinated poly(N-vinylcarbazole) (PVKI) by chemical reaction modifies considerably the photoconductive property of PVKI. The photoinduced discharge rates for pure PVK, PVKI, C-60-chemically modified PVKI (C-60-PVKI copolymer), and C-60-doped PVKI (a simple mixture of the component) under the same experimental conditions are found in the following order : C-60-PVKI copolymer > C-60-doped PVKI > PVKI > PVK. The fullerenated PVKI has a visibly brownish yellow cast when compared with the unreacted polymer. The UV-vis absorption spectrum in which the main bands occur at 220, 230, 252, 268, 300, 332, and 346 nm extends the active range from about 300 to 860 nm. Also, its apparent temperature sensitivity is very intriguing, and an unusual temperature dependence for the ESR spectrum is observed. The photoconductive performance of the fullerenated polymer is closely related to its paramagnetism. A considerable difference of electronic structure between pure PVKI and the C-60-PVKI copolymer is indicated.