We hydrothermally synthesized anatase films on Ti substrates from transparent aqueous solutions of layered titanate colloids. The morphology and wetting properties of the films were examined. The films consisted of columnar aggregates grown on the Ti substrates, which resulted in high orientation. Randomly oriented films were obtained when alumina was used as a substrate, whereas the sol-gel precoating of a titanium oxide (TiO2) layer on alumina substrates resulted in similar orientation as that of the films on Ti substrates. Thus, the presence of TiO2 on the substrate surface plays an important role in the orientation of columnar aggregates. The columnar aggregates were similar in microstructure to the arms of a type of six-pointed star-like anatase aggregate synthesized hydrothermally from the same reaction solutions. They were composed of twins of tapered anatase nanocrystals, which provided a rough film surface. The film surface was highly hydrophilic and oleophilic due to the nanoscale roughness even when the film was not irradiated with UV light.