We present a novel approach to cover different substrates with thin light-sensitive layers that consist of organic-capped TiO2 nanorods (NRs). Such NR-based coatings exhibit an increasing initial hydrophobicity with increasing NR length, and they demonstrate a surface transition from this highly hydrophobic state to a highly hydrophilic one under selective UV-laser irradiation. This behaviour is reversed under long dark storage. Infrared spectroscopy measurements reveal that light-driven wettability changes are accompanied by a progressive hydroxylation of the TiO2 surface. The surfactant molecules that cover the NRs do not appear to suffer for any significant photocatalytic degradation.