This work presents pulsed UV laser treatment (355 nm, 2 Hz) of TiO2 nanotubes decorated with chromium oxides. The modification was performed in a system equipped with a beam homogenizer, and during the irradiation, the samples were mounted onto the moving motorized table. In such a system, both precisely selected areas and any large area of the sample can be modified. Photoelectrochemical tests revealed photoresponse of laser-treated samples up to 1.37- and 18-fold under the illumination with ultraviolet-visible and visible light, respectively, in comparison to bare titania. Optimal beam energy fluence regarding sample photoresponse has been established. Scanning electron microscopy images, X-ray diffraction patterns, along with Raman and X-ray photoelectron spectra, suggest that the enhanced photoresponse results from changes solely induced in the layer of chromium oxides. It is believed that the results of the present work will contribute to a wider interest in laser modification of semiconductors exhibiting improved photoelectrochemical activity.