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A series of N-doped TiO2 nanocrystals with exposed {001} facets was prepared successfully by sol-gel method for the first time. The physicochemical properties of these resultant photocatalysts were characterized by XRD, TEM, XPS, and DRS, and their photocatalytic performances were evaluated by photocatalytic decoloration of methylene blue solution under visible light (λ>420 nm) irradiation. The results showed that the N-doped TiO2 nanocrystals with exposed {001} facets showed higher photocatalytic activity than P25. The enhanced photocatalytic performance can be attributed to synergistic effects of several factors, such as good crystallinity, better light response characteristic, and high reactivity of {001} facets.