Nitrogen-doped TiO2 has been prepared by calcining technical grade guanidine hydrochloride and commercial anatase TiO2 powders. XRD patterns indicate that the prepared powders are composed of anatase. XPS results show that N atoms have been incorporated into the lattice of anatase. UV-Vis reflectance spectra show that the light absorption of the synthesized N-doped anatase powders has red-shifted well into visible-light region. Degradation of methylene blue (MB) aqueous solution by N-doped anatase has been investigated by UV-Vis light spectrophotometer. The 400-mL 10 mg/L aqueous solution of MB could be degraded with 4 g N-doped TiO2 within 4.5 hrs of visible light irradiation. Photocatalytic paint was prepared by adding the synthesized N-doped nanocrystalline anatase TiO2 powders into self-engineered oxidation resistance latex paint system. The effects of the amount and types of the TiO2 in the paints on the sterilization were systematically investigated. The colony counting method was used to study its sterilization performance under visible light irradiation. The sterilization experiments show that the rate of sterilizing E. coli by the N-doped TiO2 modified paint can exceed more than 99% after irradiation by the visible light for 2 to 4 hours.