N-doped TiO2 nanoparticle powders were prepared efficiently by the sol-gel method using triethylamine and ammonium hydroxide as composite N precursor. The as-prepared N-doped TiO2 precursor powders were calcined at 300°C in air for 3 h and subsequently annealed at 300°C in air for 2.5 h. The samples were characterized by X-ray diffraction, transmission electron microscopy, Fourier transform infrared spectroscopy, thermo-gravimetric analysis, and X-ray photoelectron spectroscopy. The visible light photocatalytic activities of as-prepared samples were evaluated by photodecomposition of methyl orange (MO). The results show that the as-prepared samples have high visible light photocatalytic activities. Triethylamine produces the N-species doped in TiO2 lattice responsible for the high visible light photocatalytic activity. Ammonium hydroxide makes the gel of the TiO2 nanoparticles nitrided by triethylamine gelate further and facilitates significantly the centrifugation of the gel. An annealing treatment can eliminate effectively the outer N species caused by ammonium hydroxide and the surface organic residues, improve effectively crystallinity, and retain the N species caused by triethylamine.