Microbial immobilization technology is effective in improving bioremediation efficiency and heavy metal pollution. Herein, Bacillus LD513 with hexavalent chromium (Cr(VI)) tolerance was isolated and immobilized on a novel ferrous disulfide (FeS2)/iron nitride (FeN) modified hydrochar (Fe3-SNHC) prepared from waste straws. The prepared Fe3-SNHC-based LD513 (FeLD) significantly improves Cr(VI) adsorption and reduction by 31.4 % and 15.7 %, respectively, compared to LD513 alone. Furthermore, the FeLD composite system demonstrates efficient Cr(VI) removal efficiency and good environmental adaptability under different culture conditions. Microbial metabolism and electrochemical analysis indicate that Fe3-SNHC is an ideal carrier for protecting LD513 activity, promoting extracellular polymer secretion, and reducing oxidative stress. Additionally, the carrier serves as an electron shuttle that accelerates electron transfer and promotes Cr(VI) reduction. Overall, FeLD is an environmentally friendly biocomposite that shows good promise for reducing Cr(VI) contamination in wastewater treatment.