Nitrogen-doped carbon nanosheets with a developed porous structure were prepared from polyurethane foams by hydrothermal carbonization following ZnCl2 chemical activation. Scanning electron microscopy, thermogravimetric analysis, Fourier transform infrared spectroscopy, solid state 13C nuclear magnetic resonance (NMR) spectra and X-ray photoelectron spectroscopy were used to characterize the nitrogen-doped carbon nanosheet structure and composition. The removal of Cr(VI) by the N-doped carbon nanosheets was investigated. The results showed that the maximum removal capacity for chromium of 188 mg/g was found at pH=2.0 with PHC-Z-3. pH had an important effect on Cr(VI) removal and the optimal pH was 2.0. Moreover, amino groups and carboxyl groups in the nitrogen-doped carbon nanosheet played important roles in Cr(VI) removal, and promoted the reduction of Cr(VI) to Cr(III).