A low-voltage ͑Ͻ2 V, three-electrode system͒ method for the cathodic electrodeposition of fullerol ͓polyhydroxylated fullerene, C 60 ͑OH͒ n ͔ from an aqueous solution has been developed for the synthesis of thin films. Scanning electron microscopy of the electrodeposited fullerol films shows that the films are microscopically uniform; the film thickness was observed to vary linearly with the deposition charge. X-ray photoelectron spectroscopy of the C 1s peak indicates that the carbon constituents of the electrodeposited films are electronically similar to the fullerol precursor. Infrared spectroscopy ͑IRS͒ confirmed that the fullerol moiety is intact upon electrodeposition and that the films are thermally stable up to 150°C. At higher temperatures IRS data suggest there is cleavage of a ketal or hemiketal group followed by hydroxyl group cleavage. The ͑direct͒ optical bandgap obtained from UV-visible spectroscopy of the electrodeposited film was 2.6 eV.Fullerene and its derivates have been widely investigated during the last decade. The unique properties of C 60 have been thought to have potential applications in a variety of areas, including optoelectronics, catalysis, superconductivity, and medical therapeutics. Examples of specific applications that have incorporated fullerene materials are optical limiting devices, 1,2 sensors, 3 polymer-based solar cells, 4-7 and solar sensitizers for wide-bandgap materials. [8][9][10][11] Several different synthetic methods for preparing films of fullerenes and derivates have been demonstrated, including thermal evaporation, 12,13 Langmuir-Blodgett film deposition, 14-16 monolayer adsorption on metals, 17,18 self-assembly of monolayers, 8,14 solution casting, 19,20 polymer blends, 21 and sol-gel 22 methods. The major limitations of the previous synthetic methods include poor morphological control, limits on film area and substrate geometry, limits on film thickness ͑Ͻ100 nm͒, 23 and high costs associated with some of these techniques.Electrochemical deposition of C 60 or its derivates is particularly attractive because of the suitability to commercial applications. Commercial electrodeposition is relatively low-cost and has a high degree of process control. One example is cathodic electropolymerization, which has been used to synthesize fullerene-containing polymers including fullerene epoxide ͑C 60 O͒ polymers from fullerene in the presence of oxygen 24,25 and directly from C 60 O. 26,27 Fullerene derivate polymers containing metal groups such as Ir in C 60 ͕Ir͑CO͒ 2 ͖ n 28 and other metals 29,30 have also been synthesized. Various other fullerene polymers have also been electrodeposited/electropolymerized 31-34 to fabricate thin films. These methods require nonaqueous solvents and in some cases an oxygen-free electrolyte, which could make the process difficult to commercialize. Cation intercalation in the electropolymerized film has been observed in some cases, 26 which would be undesirable for certain applications. Kamat et al. 35,36 and others 37 have used electrochemi...