TiO2 hybridized with nitrogen‐doped carbon (N‐doped C/TiO2) was prepared as a photocatalyst with improved visible‐light catalytic activity for the first time. It was found that N‐doped carbon was formed by etching and partial decomposition of as‐formed graphitic carbon nitride on the surface of TiO2 under calcination at 500 °C in open air, which avoided direct doping of nitrogen into TiO2 structure. N‐doped carbon on the surface of TiO2 led to an enhanced light absorption in the range of 400 to 550 nm. The resulting N‐doped C/TiO2 exhibited about 2 times higher activity than the graphitic carbon nitride/TiO2 prepared by direct carbonization in argon atmosphere. Compared with the commercial TiO2 (Degussa, P25), N‐doped C/TiO2 showed a higher reaction rate in the degradation of various pollutants such as rhodamine B, phenol and methyl orange (MO) under simulated solar light irradiation.