Nanoscale TiO2 photocatalysts are key materials for convenient wastewater treatment and other essential cleaning processes. Immobilization of TiO2 nanoparticles (NPs) is thus indispensable for the facile handling and separation of nanocatalysts as well as for minimizing their potential health and environmental hazards. Silicone nanofilaments are introduced as a new flexible carrier type for titania NPs because they are compatible with a wide range of substrates and they display high chemical stability. TiO2-NPs are deposited on glass slides covered with thin carpets of silicone nanofilaments in a single reaction step starting from TiF4 and optimized ethanol/water ratios. The resulting composites are characterized using a wide range of electron microscopy and other analytical techniques, and their photocatalytic activity in the decomposition of methylene blue (MB) is superior to immobilized TiO2 references on plain substrates.