The g-C3N4 nanosheets with N-defects were fabricated by a sample oxidative reaction via H2O2, which can generate hydroxyl radical (•OH) to destruct the bonds of g-C3N4. The existence of •OH was confirmed by PL (photoluminescence spectroscopy) and HPIC (high-pressure ion chromatography). The N-defects were confirmed by the concentration of nitrate in solution increasing from 1.04 to 4.65 mg/L. Further, the source of N-defects was speculated as the destruction of CNC due to its lower bond-energy and decreasing ratio of CNC (CASTEP, XPS). As a result, the obtained N-defective g-C3N4 improved the photocatalytic degradation efficiency to Methylene blue (MB) from 53.1% (g-C3N4) to 100.0% under visible light. This result was ascribed by the N-defect narrowed the bandgap from 2.71 to 2.67 eV, accelerated the separation and transfer of photo-generated carriers. This work provides a new strategy to construct defects in a catalyst improving photocatalytic performance.