AbstractA technique is presented that allows for altering of the physical characteristics of films of TiO2 nanoparticles by exposure to visible light. In this technique, dye‐sensitized oxide nanoparticles are deposited on a substrate by dip‐coating. Photodissociation of the organic ligand layer leads to cross‐linking of the nanoparticles. Consequently, irradiated films have a decreased porosity, an increased index of refraction and an increased hydrophobicity. Films irradiated with green light are compared to films irradiated with UV light. Within experimental error, visible‐ and UV‐illumination induces the same changes in the films. The mechanism of surfactant elimination in dye‐sensitized oxide particles is discussed, patterning is demonstrated, and prospective applications of the technique are considered.