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We report the photoinduced conductivity changes measured on a system composed of single-wall carbon nanotubes (SWNTs) modified by a semiconducting poly(amidoamine) dendrimer (PAMAMC) characterized by highly aromatic end groups. Under illumination hole injection into SWNTs prevails over the photoinjection of electrons from PAMAMC to SWNT holes, and film photoconductivity is observed. This system was incorporated as an electroactive component within a conducting polymer [poly(3-octylthiophene)], providing improvements in the photoelectrical properties of the composite. Such supramolecular structures consisting of dendrimer-functionalized carbon nanotubes provide the means for an approach toward the preparation of photoactive materials of high current interest.