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Multi-walled carbon nanotubes (MWNTs) were functionalized via oxidative polymerization of 3-3_(vinylcarbazole) (PVK). Thin films of PVK-functionalized MWNTs (PVK-MWNTs) were fabricated by the Langmuir–Schaefer (LS) technique and characterized by spectroscopic, microscopic, electrical and electrochemical techniques before and after doping with iodine. I/V characterization showed an increase in the conductivity of the PVK-MWNTs and I2-doped PVK-MWNTs compared with the PVK and I2-doped PVK, respectively. The electrochemical characterization showed the formation of an I2-doped PVK-MWNT complex. These nanostructured PVK-MWNT films revealed an increase in the current density under illumination of about 500 nA cm−2.