In the process of water treatment, excessive nitrogen and phosphorus pollutants are of great concern. Therefore, we prepared nanoscale zero-valent iron loaded on sediment-based biochar (nZVI-SBC) to conduct nitrate and phosphate removal at the same time. The characterization demonstrated that nZVI-SBC was successfully synthesized, which had obvious advantages for larger specific surface area and better dispersion compared with pure nZVI. The batch experiments indicated that the best loading ratio of nZVI to SBC and optimum dosage for nitrate and phosphate were 1:1and 2 g·L-1, respectively. Their removal by nZVI-SBC was an acid-driven process. Anoxic environment was more conducive to the reduction of nitrate while the phosphate removal was fond of oxygen environment. 77.78% of nitrate and 99.21% of phosphate have been successfully removed, mainly depending on reduction and complexation mechanism, respectively. Moreover, nZVI-SBC had higher N2 selectivity and produced less ammonium than nZVI. The interaction between nitrate and phosphate was studied to manifest that they had different degrees of inhibition during the removal of the other. Our research indicated that nZVI-SBC has great potential for remediation of nitrogen and phosphorus polluted water.