TiO₂photocatalyst is of interest for antimicrobial coatings on hospital touch-surfaces. Recent research has focused on visible spectrum enhancement of photocatalytic activity. Here, we report TiO₂with a high degree of nanostructure, deposited on stainless steel as a solid layer more than 10 μm thick by pulsed-pressure-MOCVD. The TiO₂coating exhibits a rarely-reported microstructure comprising anatase and rutile in a composite with amorphous carbon. Columnar anatase single crystals are segmented into 15–20 nm thick plates, resulting in amille-feuillesnanostructure. Polycrystalline rutile columns exhibit dendrite generation resembling pine treestrobili. We propose that high growth rate and co-deposition of carbon contribute to formation of the unique nanostructures. High vapor flux produces step-edge instabilities in the TiO₂, and solid carbon preferentially co-deposits on certain high energy facets. The equivalent effective surface area of the nanostructured coating is estimated to be 100 times higher than standard TiO₂coatings and powders. The coatings prepared on stainless steel showed greater than 3-log reduction in viableE coliafter 4 hours visible light exposure. The pp-MOCVD approach could represent an up-scalable manufacturing route for supported catalysts of functional nanostructured materials without having to make nanoparticles.