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To address this challenge, this work presents a holistic biomimetic strategy based on the natural laccase catalytic process, designing a novel nanozyme Cu\u2010Cys@PCN\u2010222(Cu\/Fe). In this nanozyme, the incorporation of Cys and the FeTCPP into the PCN\u2010222 framework achieves the biomimicry of the substrate binding pocket and oxygen\u2010carrying hydrophobic sites, respectively. These two key components enables efficient pollutant enrichment and enhances dissolved oxygen capture and transport. Finally, Cys and TCPP within the PCN\u2010222 framework through the coordination with copper constructed the CuN\n                    <jats:sub>4<\/jats:sub>\n                    (OH\n                    <jats:sub>2<\/jats:sub>\n                    )\/Cu\u2010S unsaturated copper clusters. This structure imitates the asymmetric coordination structure of the natural laccase active center, achieving highly efficient catalysis of substrate molecules. The synergy factor confirms the synergistic interaction among the three biomimetic functions, and this synergistic architecture promotes a highly efficient catalytic cycle, endowing the nanozyme with 2.2\u2010fold higher activity than natural laccase, as well as excellent structural stability and broad substrate universality. Furthermore, the degradation mechanism and intermediate product evolution were systematically investigated. This work establishes a generalizable paradigm for designing high\u2010performance biomimetic catalysts via the holistic biomimetic strategy.\n                  <\/jats:p>","DOI":"10.1002\/smll.73924","type":"journal-article","created":{"date-parts":[[2026,5,26]],"date-time":"2026-05-26T10:29:47Z","timestamp":1779791387000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["A Holistically Engineered Laccase Nanozyme With Enhanced Activity for Phenolic Compound Removal"],"prefix":"10.1002","volume":"22","author":[{"given":"Chi","family":"Xu","sequence":"first","affiliation":[{"name":"Guangxi Key Laboratory of AI\u2010Driven Zero\u2010Carbon Technology Key Laboratory of New Low\u2010Carbon Green Chemical Technology Education Department of Guangxi Zhuang Autonomous Region School of Chemistry and Chemical Engineering Guangxi University  Nanning 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