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However, soft\u2010templating synthesis of multicomponent systems is typically constrained by poor structural control arising from phase separation, uncontrolled nucleation, and structural collapse. Inspired by biomineralization, this study proposes a biomimetic confined crystallization strategy based on constructing a 3D continuous poly(acrylic acid) matrix. This matrix forms a flexible organic\u2013inorganic network that stabilizes intermediate species, regulates crystallization kinetics, suppresses burst nucleation, and promotes integrated crystal growth, thereby playing a role analogous to the organic framework in natural biomineralization. In addition, the template directs mesostructure formation through its space\u2010occupying effect and decomposition\u2010induced gas evolution. As a result, large\u2010sized single\u2010crystalline multicomponent MMOs were successfully synthesized. More importantly, this strategy enables precise and tunable control of crystallinity and particle size and can be readily extended to more than ten multicomponent systems. As a representative example, La\n                    <jats:sub>2<\/jats:sub>\n                    FeCuO\n                    <jats:sub>6<\/jats:sub>\n                    exhibits a Faradaic efficiency of 98.2% for electrocatalytic nitrate reduction, benefiting from the synergistic effects of optimized electronic structure, mesoporosity, and single crystallinity. Overall, this work establishes a biomimetic route to overcome the intrinsic limitations of conventional soft\u2010templating approaches, particularly phase separation, polycrystallization, and the difficulty of achieving large\u2010sized crystal growth under high\u2010temperature calcination.\n                  <\/jats:p>","DOI":"10.1002\/anie.1975103","type":"journal-article","created":{"date-parts":[[2026,9,23]],"date-time":"2026-09-23T16:13:47Z","timestamp":1790180027000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Biomimetic Confined Crystallization of Large\u2010Sized Single\u2010Crystalline Multicomponent Mesoporous Metal Oxides"],"prefix":"10.1002","author":[{"given":"Luoqi","family":"Wang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry Jilin University  Changchun Jilin 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Chemicals, Liaoning Key Laboratory for Catalytic Conversion of Carbon Resources, School of Chemical Engineering Dalian University of Technology  Dalian China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiaqi","family":"Yang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry Jilin University  Changchun Jilin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zihan","family":"Wu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry Jilin University  Changchun Jilin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ye","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry Jilin University  Changchun Jilin 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