A photocatalytic thin film of TiO 2 nanoparticles and polyaniline-grafted-chitosan (CPANI) was fabricated by layer-bylayer (LbL) approach. The growth of the self-assembly of polymer nanocomposite was monitored by UV-vis spectroscopy and the thin film morphology was analyzed from scanning electron microscopy (SEM). Poly(styrene sulfonate) (PSS) was used as a bridging layer between TiO 2 nanoparticles and CPANI. Incorporation of CPANI within the LbL self-assembly of polymer nanocomposites enhanced the dye degradation ability of the thin film. These results indicate that the presence of CPANI improves the adsorption of dye in the self-assembly. The effect of surface area and the amount of catalyst was also examined. The reusability of the thin films for dye degradation study ensures the stability of the self-assembly. © 2011 American Chemical Society.