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Here, we report an electronic modulation strategy that enables cofactor\u2010free FMO\u2010like catalysis within a high\u2010entropy alloy nanozyme (HEAzyme\u2010Cu\n                    <jats:sub>1.5<\/jats:sub>\n                    ). We induce localized electron cloud enrichment that shifts Cu 3\n                    <jats:italic>d<\/jats:italic>\n                    orbitals toward the Fermi level, establishing a self\u2010sustained redox channel without flavin cofactors. This atomic\u2010scale entropy\u2010driven alignment bridges the functional gap between natural cofactor\u2010dependent enzymes and artificial catalysts, demonstrating for the first time that complex redox cascades traditionally confined to biological systems can be reconstructed purely by materials design. This entropy\u2010driven electronic reconfiguration enables near\u2010zero barrier O\n                    <jats:sub>2<\/jats:sub>\n                    activation and rapid hydroxylation with a kinetic constant. Integrating this multifunctional HEAzyme into a portable hydrogel sensor platform achieves real\u2010time antibiotic detection down to 11\u201325\u00a0nM and &gt;\u00a090% degradation within 20\u00a0min in complex water samples. This work establishes a universal design principle for programmable enzyme mimetics, where atomic\u2010scale entropy, electronic\u2010state alignment, and multimetal cooperation converge to emulate and transcend biological catalysis. Such entropy\u2010encoded redox systems offer a transformative route toward intelligent bioinspired materials for environmental remediation, green synthesis, and metabolic engineering.\n                  <\/jats:p>","DOI":"10.1002\/adma.74827","type":"journal-article","created":{"date-parts":[[2026,8,27]],"date-time":"2026-08-27T11:25:26Z","timestamp":1787829926000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Entropy\u2010Encoded Electronic Reconstruction in High\u2010Entropy Nanozymes Enables Cofactor\u2010Free Monooxygenase\u2010Like Catalysis"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-6640-0427","authenticated-orcid":false,"given":"Xiaodi","family":"Niu","sequence":"first","affiliation":[{"name":"College of Food Science and Engineering Jilin University  Changchun P.R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hongsu","family":"Wang","sequence":"additional","affiliation":[{"name":"College of Food Science and Engineering Jilin University  Changchun P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,8,27]]},"reference":[{"key":"e_1_2_10_2_1","doi-asserted-by":"publisher","DOI":"10.31764\/jmm.v8i6.27047"},{"key":"e_1_2_10_3_1","doi-asserted-by":"publisher","DOI":"10.15666\/aeer\/1905_39593977"},{"key":"e_1_2_10_4_1","volume-title":"Innovations in Food Technology: Current Perspectives and Future Goals","author":"Singh A.","year":"2020"},{"key":"e_1_2_10_5_1","doi-asserted-by":"publisher","DOI":"10.1080\/03067319.2021.1912330"},{"key":"e_1_2_10_6_1","first-page":"63","article-title":"A Review of the Stability of Antibiotic Residues in Animal Products During Food Processing","volume":"1","author":"Al\u2010Mahmood O. 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