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Immune modulation plays a crucial role in heart valve regeneration by reversing the coagulation and inflammatory microenvironment, thereby facilitating recellularization. In this study, a biosynthesis factory is constructed on decellularized heart valves (DHVs) to continuously convert the abundant heme in the blood into immunomodulators, supporting long\u2010term immune modulation and tissue regeneration. This biosynthesis factory is achieved through a grafting from DNA hydrogel, utilizing tailored rolling circle amplification (RCA) on DHVs. Anti\u2010coagulation NU172 aptamers are incorporated into the DNA hydrogel to recruit heme from the bloodstream, while heme oxygenase 1 (HO\u20101) is encapsulated to simultaneously convert heme into biliverdin. This system ensures the sustained production of biliverdin, facilitating anti\u2010inflammatory immune modulation and reactive oxygen species (ROS) scavenging, thus creating a regenerative immune microenvironment. Additionally, the DNA coating is further crosslinked with zwitterionic polymers, which protect the functional DNA layer and provide anti\u2010calcification and anti\u2010adhesion properties. This comprehensive design promotes full endothelial cell coverage and significant extracellular matrix remodeling within one\u2010month post\u2010implantation.<\/jats:p>","DOI":"10.1002\/adma.202506728","type":"journal-article","created":{"date-parts":[[2025,6,13]],"date-time":"2025-06-13T01:25:23Z","timestamp":1749777923000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["Constructing Immunomodulator Biosynthesis Factory in Grafting\u2010From DNA Hydrogel for Heart Valve Regeneration"],"prefix":"10.1002","volume":"37","author":[{"given":"Jinsheng","family":"Li","sequence":"first","affiliation":[{"name":"Department of Cardiovascular Surgery Union Hospital Tongji Medical College Huazhong University of Science and Technology  1277 Jiefang Avenue Wuhan 430022 China"},{"name":"Hubei Engineering Research Center for Biomaterials and Medical Protective Materials Hubei Key Laboratory of Bioinorganic Chemistry &amp; Materia Medica State Key Laboratory of Materials Processing and Die &amp; 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