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We report FibrilPaints, a family of modular peptides designed for amyloid binding and adaptable chemical functionality. The degenerative amyloid\u2010targeting unit of FibrilPaints, W5P4H3R2, has a high content of \u03c0\u2010stacking and aromatic side chains. Systematic sequence variation, altering charge, termini, and residue order, revealed the importance of the composition of the amyloid\u2010targeting unit for high\u2010affinity binding across Tau and Huntingtin fibrils. Importantly, sequence changes outside this unit do not preclude fibril binding, which permits attachment of fluorophores or E3\u2010recruiting motifs for targeted protein degradation. This work establishes FibrilPaint as a modular peptide system for binding Tau and Huntingtin amyloid fibrils, with potential for broader detection and modulation applications.<\/jats:p>","DOI":"10.1002\/chem.71539","type":"journal-article","created":{"date-parts":[[2026,8,5]],"date-time":"2026-08-05T13:05:00Z","timestamp":1785935100000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Fibrilpaint: A Class of Amyloid\u2010Targeting Peptides"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1991-3283","authenticated-orcid":false,"given":"J\u00falia","family":"Aragon\u00e8s Pedrola","sequence":"first","affiliation":[{"name":"Cellular Protein Chemistry, Bijvoet Center for Biomolecular Research Utrecht University  Utrecht The Netherlands"},{"name":"Science for Life Utrecht University  Utrecht The Netherlands"},{"name":"Protein Chemistry of Disease, Department of Chemistry Utrecht University  Utrecht The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0004-6482-8082","authenticated-orcid":false,"given":"Fran\u00e7oise A.","family":"Dekker","sequence":"additional","affiliation":[{"name":"Cellular Protein Chemistry, Bijvoet Center for Biomolecular Research Utrecht University  Utrecht The Netherlands"},{"name":"Science for Life Utrecht University  Utrecht The Netherlands"},{"name":"Protein Chemistry of Disease, Department of Chemistry Utrecht University  Utrecht The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Katrin","family":"Guttmann","sequence":"additional","affiliation":[{"name":"Protein Chemistry of Disease, Department of Chemistry Utrecht University  Utrecht The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-9638-2551","authenticated-orcid":false,"given":"Litske M.","family":"van Leeuwen","sequence":"additional","affiliation":[{"name":"Science for Life Utrecht University  Utrecht The Netherlands"},{"name":"Protein Chemistry of Disease, Department of Chemistry Utrecht University  Utrecht The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0017-3281","authenticated-orcid":false,"given":"Shalini","family":"Singh","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Edmond J. Safra Campus at Givat Ram The Hebrew University of Jerusalem Jerusalem Israel"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guy","family":"Mayer","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Edmond J. Safra Campus at Givat Ram The Hebrew University of Jerusalem Jerusalem Israel"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tommaso","family":"Garfagnini","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Edmond J. Safra Campus at Givat Ram The Hebrew University of Jerusalem Jerusalem Israel"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1592-1278","authenticated-orcid":false,"given":"Assaf","family":"Friedler","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Edmond J. Safra Campus at Givat Ram The Hebrew University of Jerusalem Jerusalem Israel"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Stefan G. D.","family":"R\u00fcdiger","sequence":"additional","affiliation":[{"name":"Cellular Protein Chemistry, Bijvoet Center for Biomolecular Research Utrecht University  Utrecht The Netherlands"},{"name":"Science for Life Utrecht University  Utrecht The Netherlands"},{"name":"Protein Chemistry of Disease, Department of Chemistry Utrecht University  Utrecht The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,8,5]]},"reference":[{"key":"e_1_2_9_2_1","doi-asserted-by":"publisher","DOI":"10.1146\/annurev\u2010biochem\u2010061516\u2010044518"},{"key":"e_1_2_9_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/nrm3810"},{"key":"e_1_2_9_4_1","doi-asserted-by":"crossref","first-page":"249","DOI":"10.1080\/13506129.2024.2405948","article-title":"Amyloid Nomenclature 2024: Update, Novel Proteins, and Recommendations by the International Society of Amyloidosis (ISA) Nomenclature Committee","volume":"31","author":"Buxbaum J. 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