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After treatment, excess heparin needs to be removed to circumvent side effects and recover the blood\u2010clotting cascade. Most existing heparin antidotes rely on direct heparin binding and complexation, yet selective compartmentalization and sequestration of heparin would be beneficial for safety and efficiency. However, such systems have remained elusive. Herein, a semipermeable protein\u2010based microcompartment (proteinosome) is loaded with a highly positively charged chitosan derivative, which can induce electrostatics\u2010driven internalization of anionic guest molecules inside the compartment. Chitosan\u2010loaded proteinosomes are subsequently employed to capture heparin, and an excellent heparin\u2010scavenging performance is demonstrated under physiologically relevant conditions. Both the highly positive scavenger and the polyelectrolyte complex are confined and shielded by the protein compartment in a time\u2010dependent manner. Moreover, selective heparin\u2010scavenging behavior over serum albumin is realized through adjusting the localized scavenger or surrounding salt concentrations at application\u2010relevant circumstances. In vitro studies reveal that the cytotoxicity of the cationic scavenger and the produced polyelectrolyte complex is reduced by protocell shielding. Therefore, the proteinosome\u2010based systems may present a novel polyelectrolyte\u2010scavenging method for biomedical applications.<\/jats:p>","DOI":"10.1002\/smll.202201790","type":"journal-article","created":{"date-parts":[[2022,5,16]],"date-time":"2022-05-16T05:00:09Z","timestamp":1652677209000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":8,"title":["A Synthetic Protocell\u2010Based Heparin Scavenger"],"prefix":"10.1002","volume":"19","author":[{"given":"Qing","family":"Liu","sequence":"first","affiliation":[{"name":"Wenzhou Institute University of Chinese Academy of Sciences (WIUCAS)  Wenzhou Zhejiang 325001 China"},{"name":"Biohybrid Materials Department of Bioproducts and Biosystems Aalto University  Espoo 02150 Finland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuo","family":"Yang","sequence":"additional","affiliation":[{"name":"Laboratory of Chemical Biology Department of Biomedical Engineering Computational Biology Group Department of Biomedical Engineering and Institute for Complex Molecular Systems Eindhoven University of Technology  Eindhoven MB 5600 The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Iris","family":"Seitz","sequence":"additional","affiliation":[{"name":"Biohybrid Materials Department of Bioproducts and Biosystems Aalto University  Espoo 02150 Finland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Anna\u2010Maria Makri","family":"Pistikou","sequence":"additional","affiliation":[{"name":"Laboratory of Chemical Biology Department of Biomedical Engineering Computational Biology Group Department of Biomedical Engineering and Institute for Complex Molecular Systems Eindhoven University of Technology  Eindhoven MB 5600 The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tom F. 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