Noble metal particles of Au, Pt, and Ir were deposited on nanostructured TiO2 film using an electrophoretic approach. The nanocomposite films were characterized by UV-absorption and atomic force microscopy (AFM). The deposition of tetraoctylammonium bromide (TOAB)-capped metal nanoparticles on TiO2 films improved the photocurrent generation and induced a shift in the apparent flat band potential. The TiO2 films modified with TOAB-capped metal nanoparticles were less prone to the electron scavenging by the oxygen in solution. Improved photoelectrochemical performance of semiconductor-metal composite film is attributed to the shift in quasi-Fermi level of the composite to more negative potentials. Continuous irradiation of the composite films over a long period causes photocurrent to decrease as the semiconductor-metal interface undergoes chemical changes. The role of semiconductor-metal composite films in improving the rate of photocatalytic degradation of an azo dye is also discussed.