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Here, we report the modular assembly of a self\u2010supporting biocatalytic material for stereoselective C\u2500Si bond formation using an engineered\n                    <jats:italic>Rhodothermus marinus<\/jats:italic>\n                    cytochrome c (CC). The material was constructed by site\u2010specific covalent coupling of CC fused with two SpyCatcher domains (SC\u2010CC\u2010SC) with streptavidin variants bearing SpyTag domains (STV\u2010ST), yielding a red, porous enzyme foam with defined hexagonal architecture. The modular STV\u2010mediated crosslinking strategy enables the formation of carrier\u2010free materials with high enzyme density and minimal diffusion barriers. The CC foams retained structural integrity and catalytic activity after drying, catalyzing the formation of a chiral organosilicon compound with high enantioselectivity under mild conditions. The enzyme remains active at the extensive gas\u2013liquid interfaces within the foam, effectively combining high catalyst loading with excellent mass transport. The resulting material retains high stereoselectivity (&gt;95% ee), exhibits catalytic performance comparable to previously reported carrier\u2010based immobilization approaches, and maintains catalytic activity over five consecutive reuse cycles. This immobilization concept establishes a generalizable platform for fabricating biocatalytic materials from monomeric enzymes and expands the scope of enzymatic C\u2500Si bond formation toward scalable, sustainable synthesis.\n                  <\/jats:p>","DOI":"10.1002\/chem.71776","type":"journal-article","created":{"date-parts":[[2026,10,7]],"date-time":"2026-10-07T09:26:41Z","timestamp":1791365201000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Modular Assembly of a Biocatalytic Material for Stereoselective C\u2500Si Bond Formation"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0001-4848-9429","authenticated-orcid":false,"given":"Marc F.","family":"M\u00fcnker","sequence":"first","affiliation":[{"name":"Institute For Biological Interfaces 1 (IBG\u20101) Karlsruhe Institute of Technology (KIT)  Eggenstein\u2010Leopoldshafen 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