This study presents a biomimetic approach for the efficient immobilization of elemental mercury (Hg⁰) using selenium-functionalized polyphenylene sulfide (PPS) fabric. The method is inspired by the biological detoxification of mercury, where selenium preferentially converts mercury from sulfoproteins to HgSe. The PPS fabric, rich in sulfur, acts as a transporter for Hg⁰, which then migrates to adjacent selenium sites for permanent immobilization. The sulfur-selenium pair provides high Hg⁰ adsorption capacity and uptake rate, reaching 1621.9 mg g⁻¹ and 1005.6 μg g⁻¹ min⁻¹, respectively, which are the highest recorded values among various materials. The in situ synthetic method for preparing Se/PPS-I fabric ensures a high density of available selenium ligands, enhancing Hg⁰ adsorption. The fabric's structure, with a tangled network of fibers, provides continuous transport channels for mercury migration to selenium sites. The study demonstrates that the selenium ligands, with high activity and accessibility, can be simultaneously constructed to provide an ideal Hg⁰ adsorbent. The Se/PPS-I fabric exhibits excellent thermal stability, pore structure, crystallinity, and surface chemistry, making it suitable for long-term use in industrial flue gas treatment. The fabric's resistance to flue gas interference and mercury recovery capabilities make it suitable for real-world applications in cleaning industrial flue gases. The study also reveals the reaction mechanism for Hg⁰ adsorption on Se/PPS-I, showing the migration of mercury from sulfur to selenium and the formation of stable HgSe. The results indicate that the Se/PPS-I fabric is a promising adsorbent for Hg⁰ removal, with high adsorption capacity and rate, and the ability to recover mercury and selenium. The study provides a biomimetic design for advanced functional filters for pollutant abatement.This study presents a biomimetic approach for the efficient immobilization of elemental mercury (Hg⁰) using selenium-functionalized polyphenylene sulfide (PPS) fabric. The method is inspired by the biological detoxification of mercury, where selenium preferentially converts mercury from sulfoproteins to HgSe. The PPS fabric, rich in sulfur, acts as a transporter for Hg⁰, which then migrates to adjacent selenium sites for permanent immobilization. The sulfur-selenium pair provides high Hg⁰ adsorption capacity and uptake rate, reaching 1621.9 mg g⁻¹ and 1005.6 μg g⁻¹ min⁻¹, respectively, which are the highest recorded values among various materials. The in situ synthetic method for preparing Se/PPS-I fabric ensures a high density of available selenium ligands, enhancing Hg⁰ adsorption. The fabric's structure, with a tangled network of fibers, provides continuous transport channels for mercury migration to selenium sites. The study demonstrates that the selenium ligands, with high activity and accessibility, can be simultaneously constructed to provide an ideal Hg⁰ adsorbent. The Se/PPS-I fabric exhibits excellent thermal stability, pore structure, crystallinity, and surface chemistry, making it suitable for long-term use in industrial flue gas treatment. The fabric's resistance to flue gas interference and mercury recovery capabilities make it suitable for real-world applications in cleaning industrial flue gases. The study also reveals the reaction mechanism for Hg⁰ adsorption on Se/PPS-I, showing the migration of mercury from sulfur to selenium and the formation of stable HgSe. The results indicate that the Se/PPS-I fabric is a promising adsorbent for Hg⁰ removal, with high adsorption capacity and rate, and the ability to recover mercury and selenium. The study provides a biomimetic design for advanced functional filters for pollutant abatement.