a b s t r a c tPerovskite-type La 2 Ti 2 O 7 (LTO), having a layered structure and the separated H 2 and O 2 evolution sites, is attractive as an efficient photocatalyst. However, the photocatalytic activity is often limited by the poor electron mobility. This problem can be conquered by hybridization with materials having efficient properties for the visible light absorption and charge carrier transport. Here, we report a two-dimensional (2D) layered composite hybridized by approximately 2 nm thick graphitic C 3 N 4 nanosheets (g-C 3 N 4 ) and 7 nm thick nitrogen doped LTO nanosheets (NLTO) (g-C 3 N 4 /NLTO), in which g-C 3 N 4 and NLTO act as hole receptor and electron conductor, respectively. g-C 3 N 4 /NLTO exhibited high photocatalytic activities for H 2 production via water splitting and dye degradation under the UV and visible light irradiation, due to the interfacial charge transfer between g-C 3 N 4 and NLTO. The electrochemical measurement showed the type II band alignment with favorable charge transfer from g-C 3 N 4 to NLTO. The 2D architecture with a maximized interfacial area allows efficient charge separation with a short interfacial distance. This efficient interfacial charge transfer is further elucidated from monitoring of charge separation and trapping processes using the femtosecond time-resolved diffused reflectance (TDR) measurement.