In this paper, an unavoidable thermodynamic behavior of nanomaterials is prevented by using a simple chemical morphology freezing method. Titanate nanotubes (no photoactivity) are filled with LaMer-model carbon and then coated with a silica sheath. This chemical filling and coating process ‘isolates’ micro-thermal deformation from the system, and consequently prevents the destruction of the tubular morphology during the calcination process. After calcination, novel high photoactivity TiO2nanotubes are obtained with perfect open-ended tubular morphology and fine anatase phase. The sample shows the highest photoactivity of all the samples, which is 2 times higher than that of TiO2nanorods, and is 4 times higher than TiO2nanoparticles (P-25).