A series of nitrogen-doped and undoped TiO2 nanocrystals was prepd. by several simple methods. Needle-like N-doped TiO2 nanocrystals and nanoparticles were obtained from com. TiO2 powders. Several dye-sensitized solar cells (DSCs) were fabricated based on N-doped and undoped TiO2 electrodes. The N-doped DSCs achieved a high conversion efficiency of 10.1% and 4.8% using an org. electrolyte and an ionic liq. electrolyte, resp. Systemic investigations were carried out on the properties of N-doped and undoped TiO2 powders, films, and DSCs. The electron transport time and electron lifetime were investigated by intensity-modulated photocurrent and photovoltage spectroscopy (IMPS/IMVS). Moreover, the electron injection of N-doped DSCs was studied by surface photovoltage spectroscopy (SPS). The synergetic effect of higher dye uptake, faster electron transport and higher photovoltage contributes to a higher conversion efficiency of N-doped DSCs. The stability test also demonstrated that the photodegrdn. of the DSCs was not accelerated and the DSC system was stabilized by the introduction of nitrogen into the TiO2 photoelectrode. These results indicate that the N-doped TiO2 nanocrystals prepd. by our approach from com. TiO2 are ideal semiconductor materials for DSCs.