Using electrophoresis for TiO2 coating and photoexcited electrons for metal-nanoparticle deposition, a facile method for the development of aligned coaxial nanowires of carbon nanotubes sheathed with TiO2 (see figure), and well-defined TiO2 nanomembranes decorated with and without metal nanoparticles, is developed. The TiO2-based nanostructures show fast photocurrent responses and possess unique photoinduced electron-transfer properties.