The mitigation of nitrogen loads from sediments is crucial for the fundamental restoration of urban lakes. As promising materials, the effectiveness of zero-valent iron (ZVI) and biochar (BC) in sediment nitrogen removal was investigated through 200-day microcosm experiments in this study. The combined application of ZVI and BC increased sediment total nitrogen (TN) and organic matter (OM) removal efficiency by 16.05 % and 6.73 %, respectively, compared to the blank. They led to an increase in chemical oxygen demand (COD) concentrations by 8.68 – 12.96 mg/L in the overlying water and 9.21 – 9.46 mg/L in the interstitial water compared to the blank. The results of the structural equation model (SEM) indicated that the addition of materials could influence overlying water dissolved oxygen, sediment oxidation-reduction potential, and sediment TN content, thus impacting nitrogen and COD concentrations in the overlying and the interstitial waters. The microbial analysis further demonstrated that ZVI coupled with BC increased the abundance of nitrifying (Methylocystis, Ellin6067), heterotrophic denitrifying (Anaerolineaceae, Steroidobacteraceae, Candidatus Competibacter), autotrophic denitrifying (Dechloromonas), and iron-oxidizing bacteria (Crenothrix). Conclusively, ZVI and BC enhanced sediment nitrogen removal by promoting heterotrophic denitrification.