AbstractIn this work, the preparation of regular nanosized columnar structures of titanium dioxide by means of glancing angle deposition with magnetron sputtering (MS‐GLAD) followed by thermal annealing is reported. MS‐GLAD gives rise to metallic titanium columnar structures with regular width and length that after thermal treatment are fully oxidized to form TiO₂ nanocolumns that maintain the morphological features of the original metallic ones. Further functionalization with gold by means of multiple ion cluster source results in well‐dispersed Au nanoparticles across the nanocolumns’ surface with a narrow size distribution centered at ca. 8.5 nm. The obtained nanostructures show photocatalytic self‐cleaning activity as shown by the elimination of an organic layer deposited on their surface and the detection of hydroxyl radicals. Photoelectrochemical measurements show a better charge separation at the Au/TiO₂ interface. In addition, wettability studies show that the degree of hydrophobicity of the surface is increased by the presence of nanocolumns, both in the dark and under UV illumination. This behavior is not modified by the presence of Au nanoparticles on the surface. The obtained results open up interesting implications in the tunability of the properties of nanostructured thin films for this kind of photo‐activated application.