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This research specifically focused on the development of a novel methodology to reduce excess nitrate in drinking water utilizing zerovalent iron nanoparticles (nZVI)-stabilized radiation-grafted copolymer matrix. nZVI was synthesized by borohydrate reduction of FeCl3 and stabilized on acrylic acid (AAc)-grafted non-woven polyethylene/polypropylene (NWPE/PP-g-AAc) copolymer matrix, which was grafted using gamma radiation. The use of nZVI for environmental applications is challenging because of the formation of an oxide layer rapidly in the presence of oxygen. Therefore, radiation-grafted NWPE/PP synthetic fabric was used as the functional carrier to anchor nZVI and enhance its spreading and stability. The chemical reduction of nitrate by nZVI-adsorbed NWPE/PP-g-AAc (nZVI-Ads-NWP) fabric was examined in batch experiments at different pH values. At low pH values, the protective layers on nZVI particles can be readily dissolved, exposing the pure iron particles for efficient chemical reduction of nitrate. After about 24 h, at pH 3, almost 96% of nitrate was degraded, suggesting that this reduction process is an acid-driven, surface-mediated process. The nZVI-water interface has been characterized by the 1-pK Basic Stern Model (BSM). An Eley-Rideal like mechanism well described the nitrate reduction kinetics. In accordance with green technology, the newly synthesized nZVI-Ads-NWP has great potential for improving nitrate reduction processes required for the drinking water industry.