Both opaque and transparent TiO2 nanocrystalline thin films were developed on glass substrates by applying dip coating and doctor-blade deposition techniques, using titanium(IV) butoxide and Degussa P25 TiO2 powder as precursor and starting material, respectively. Atomic force microscopy (AFM) and scanning electron microscopy (SEM) evaluated the surface characteristics of the films. Results on their structure and crystallinity were obtained by means of X-ray diffraction and Raman spectroscopy. The catalytic activity of the films towards photodegradation of 3,5-dichlorophenol (3,5-DCP) pollutant was examined and their efficiency was compared to that of the TiO2 powder (slurry) suspensions. Pseudo-first-order photodegradation kinetics were observed and the reaction constants were determined. It has been shown that the film photocatalysts can efficiently decompose the pollutant, although relatively higher decomposition rates were observed with the commercial starting powder. Differences in the film efficiencies can be attributed to differences in their grain size, surface roughness and fractal parameters. No altering on the doctor-blade films surface characteristics was observed for several hours of cyclic operation during which their photocatalytic efficiency remained remarkably stable.