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However, reproducing the exquisite selectivity of enzymatic catalysis, particularly their ability to operate with high precision in complex reaction systems, remains a central challenge. Herein, inspired by the heme\u2013pocket architecture and cooperative regulation in cytochrome P450, we report a nanozyme multilevel programming strategy based on a single\u2010atom covalent organic framework (COF) platform constructed from heme\u2010like metal\u2013porphyrin nodes and linkers bearing chiral amino\u2010acid residues, enabling selective editing of metal catalytic centers and enzyme\u2010mimetic pockets to control catalytic activity, chemoselectivity, and stereochemical outcomes. As a proof of concept, we employ a biomimetic chiral cascade that couples methanol dehydrogenase\u2010like alcohol oxidation with a chymopapain\u2011inspired asymmetric aldol reaction to probe and optimize metal\u2013pocket cooperativity within the nanozyme. The programmed MnPor\u2010Pro\u2010based nanozyme delivers high product yields, excellent chemo\u2010 and stereoselectivity, and outstanding recyclability in the cascade reactions, indicating the effectiveness of this strategy. This work provides a rational design insight for engineering highly selective nanozymes capable of addressing complex, multistep transformations, significantly bridging the gap between artificial and natural enzymatic systems.<\/jats:p>","DOI":"10.1002\/adma.74678","type":"journal-article","created":{"date-parts":[[2026,8,21]],"date-time":"2026-08-21T11:32:54Z","timestamp":1787311974000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Engineering Metal\u2010Pocket Cooperativity in Single\u2010Atom COF Nanozymes for Selective Cascade Catalysis"],"prefix":"10.1002","volume":"38","author":[{"given":"Ziping","family":"Li","sequence":"first","affiliation":[{"name":"School of Chemical Engineering and Australian Centre For NanoMedicine The University of New South Wales  Sydney New South Wales 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