Electrochemical polymerization of N-vinyl carbazole (VK) on carbon nanotube (CN) films was studied by cyclic voltammetry in LiClO4/acetonitrile solutions. Cyclic voltammograms recorded on a blank Pt electrode were compared with those obtained when single or multi-walled CN films were deposited on the Pt electrode; in the latter case, a down-shift of the VK reduction peak potential was observed. Functionalization of CNs with poly(N-vinyl carbazole) (PVK) was invoked by Raman scattering and UV-VIS-NIR spectroscopic studies. The influence of sweep rate on the electrochemical properties of the PVK/CN nanocomposite and the performance of supercapacitors constructed using PVK-functionalized single-walled carbon nanotube electrodes were also evaluated.