To solve the problem of heavy metal hexavalent chromium (Cr(VI)) pollution in water bodies, this study was carried out to prepare nitrogen-doped porous carbon by using bamboo shoots as the raw material and KHCO3 as the activator, which has a good ability to remove Cr(VI) from water bodies. The prepared N-doped carbon materials were characterized by thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FT-IR), elemental analysis, and scanning electron microscopy (SEM). The results showed that the prepared carbon material had hierarchical pore structures and abundant functional groups, which is conducive to the adsorption of Cr(VI). The effects of various factors on the adsorption performance of Cr(VI), such as the carbon materials prepared under different conditions, the pH of the initial solution, the concentration of the initial solution, and the contact time between the carbon and Cr(VI), were explored. The results showed that the bamboo shoot-based nitrogen-doped carbon materials, especially BSNC-800 (prepared at 800 °C with a mass ratio of KHCO3 to bamboo shoot of 4:1), performed well in removing Cr(VI) from a water solution. The maximum adsorption of Cr(VI) by BSNC-800 under equilibrium conditions was 385.8 mg g−1 (conditions: at the pH of 2 with the initial concentration of 400 mg L−1). The adsorption kinetics and isotherms were analyzed, and the adsorption mechanism was discussed. It can be found that the adsorption of Cr(VI) by BSNC-800 fits better with the Langmuir isotherm model and the pseudo-second-order kinetic model. The adsorption mechanism between the Cr(VI)-containing solution and BSNC-800 was controlled by membrane diffusion and chemisorption. The results broaden the ways of utilizing biomass resources as precursors of carbon materials, which is significant and helpful for applying biomass carbon materials as adsorbents for wastewater treatment.