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Both doping and compositing in TiO 2 are exceedingly effective strategies to overcome the compound's shortcomings, such as invalid visible-light response and enormous recombination of photogenerated carriers. Herein, a convenient and costeffective route has been put forward to in situ synthesize nanolayered heterostructure based on N-doped TiO 2 nanoparticles and Ndoped carbon (N-TiO 2 /NC) using 2D layered N-MXene (N−Ti 3 C 2 T x ) as the template. The as-obtained N-TiO 2 /NC nanocomposite displays greatly enhanced visible light absorption property, superior carrier separation and transport ability. As a result, the nanolayered N-TiO 2 /NC heterostructure exhibits a satisfactory H 2 evolution rate from water-splitting (102.6 μmol g −1 h −1 ) under visible-light without any additional cocatalyst. The study provides a new strategy for the synthesis of defective nanoheterostructure and expands the applications of MXene family.