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Replicating these capabilities in common protein systems remains challenging, especially in stabilizing hydrophobic residues at interface and improving cohesive properties. Here, we developed unfolded protein\u2010based adhesives via a universal strategy of locking with polyelectrolytes that have flexible long chains and high charge density. These polyelectrolytes simultaneously stabilize exposed hydrophobic residues on the unfolded proteins and reinforce cohesion properties via chain entanglement with electrostatic\/hydrogen bonding interactions. The unfolded bovine serum albumin (UBSA) and polyacrylic acid (PAA) are integrated to prepare a representative tissue adhesive (UBSA\u2010PAA), exemplifying the polyelectrolyte\u2010locking strategy. The UBSA\u2010PAA adhesive demonstrated interfacial hydrophobicity (water contact angles &gt;90\u00b0) and excellent adhesion performance on wet tissue. In severe liver and femoral artery hemorrhage models, this adhesive significantly reduced blood loss compared to commercial fibrin glue, while maintaining comparable biocompatibility. This polyelectrolyte\u2010locking molecular engineering strategy provides a universal framework for designing protein\u2010based adhesives with excellent wet adhesion performance.<\/jats:p>","DOI":"10.1002\/adma.202511921","type":"journal-article","created":{"date-parts":[[2025,12,23]],"date-time":"2025-12-23T07:02:42Z","timestamp":1766473362000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":7,"title":["A Universal Polyelectrolyte\u2010Locking Strategy: From Common Proteins to Stable Unfolded Protein\u2010Based Adhesives for Rapid and Robust Tissue Sealing"],"prefix":"10.1002","volume":"38","author":[{"given":"Ruifen","family":"Yang","sequence":"first","affiliation":[{"name":"MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ruilin","family":"Shang","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiayan","family":"Hu","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zongrui","family":"Tong","sequence":"additional","affiliation":[{"name":"Key Laboratory of Precision Diagnosis and Treatment for Hepatobiliary and Pancreatic Tumor of Zhejiang Province Department of Hepatobiliary and Pancreatic Surgery The Second Affiliated Hospital School of Medicine Zhejiang University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1335-0125","authenticated-orcid":false,"given":"Lisha","family":"Yu","sequence":"additional","affiliation":[{"name":"Key Laboratory of Precision Diagnosis and Treatment for Hepatobiliary and Pancreatic Tumor of Zhejiang Province Department of Hepatobiliary and Pancreatic Surgery The Second Affiliated Hospital School of Medicine Zhejiang University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7990-2856","authenticated-orcid":false,"given":"Zhengwei","family":"Mao","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University  Hangzhou China"},{"name":"Key Laboratory of Precision Diagnosis and Treatment for Hepatobiliary and Pancreatic Tumor of Zhejiang Province Department of Hepatobiliary and Pancreatic Surgery The Second Affiliated Hospital School of Medicine Zhejiang University  Hangzhou China"},{"name":"State Key Laboratory of Transvascular Implantation Devices  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,12,22]]},"reference":[{"key":"e_1_2_9_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.3c00380"},{"key":"e_1_2_9_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/nmat4463"},{"key":"e_1_2_9_4_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202414092"},{"key":"e_1_2_9_5_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.adg4031"},{"key":"e_1_2_9_6_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.abm9744"},{"key":"e_1_2_9_7_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201704847"},{"key":"e_1_2_9_8_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010019\u201013312\u20100"},{"key":"e_1_2_9_9_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.aba6112"},{"key":"e_1_2_9_10_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.aaz9531"},{"key":"e_1_2_9_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202413171"},{"key":"e_1_2_9_12_1","article-title":"Sequential\u2010Crosslinking Fibrin Glue for Rapid and Reinforced Hemostasis","volume":"11","author":"Yu L. 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