Nitrogen-doped TiO2 nanocrystalline powders were prepared by hydrolysis of tetrachloride titanium (TiCl4) in a mixed solution of ethanol and ammonium nitrate (NH4NO3) at ambient temperature and atmosphere followed by calcination at 400 C for 2 h in air. FTIR spectra demonstrate that amine group in original gel is eliminated by calcination, and the TiO2 powder is liable to absorb water onto its surface and into its capillary pore. XRD and SEM results show that the average size of nanocrystalline TiO2 particles is no more than 60 nm and with increasing the calcination temperature, the size of particles increases. XPS studies indicate the nitrogen atom enters into the TiO2 lattice and occupies the position of oxygen atom. The nitrogen doping not only depresses the grain growth of TiO2 particles, but also reduces the phase transformation temperature of anatase to rutile. The photocatalytic activity of the nitrogen-doped TiO2 powders has been evaluated by experiments ofphotocatalytic degradation aqueous methylene blue.