N-doped Li4Ti5O12 nanosheets (NLTO) have been prepared by a simple hydrothermal reaction with further heat treatment at low temperature (500 °C) under NH3 atmosphere. The effects of the Nitrogen on structure and electrochemical performance are extensively studied. XRD results show that nitrogen doping does not change the Li4Ti5O12 (LTO) crystal structure. TEM and SEM results indicate the as-synthesized NLTO has an irregular nano-sheet-like structure with a size of 50–200 nm, which results in short Li+ diffusion paths and rapid charge transfer reactions due to the high electrode–electrolyte interface area. Galvanostatic charge–discharge tests show that NLTO exhibits a higher rate capability of 151.8 mAh g−1 at 10 C than that of LTO (139.1 mAh g−1 at 10 C), suggesting that N-doping is beneficial to the improvement in high-rate capability of the Li4Ti5O12 nanosheets.