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We report a peptide\u2013polyethylene glycol (PEG) multiblock copolymer (MBCP) using the amphipathic \u03b2-sheet-forming SAP K(FEFK)2K as a physical cross-linker. Synthesized via copper-free strain-promoted azide\u2013alkyne cycloaddition (SPAAC), the MBCP was solution-cast from water into free-standing films whose properties were governed by the peptide\u2019s ability to form stable \u03b2-sheet fibers and aggregates. Films were tough and plastic at room temperature, but elastomeric above PEG\u2019s melting point (&amp;gt;60 \u00b0C). At high temperature, a micro- and nano-scale phase-separated morphology emerged, with peptide fiber-rich domains embedded in a soft, amorphous PEG matrix. At room temperature, only microphase separation persisted, while PEG crystallization produced a semicrystalline matrix in which peptide fibers restricted large crystal growth and were likely segregated at crystallite interfaces. Extensive mechanical testing revealed resilient films with shape-recovery behavior.<\/jats:p>","DOI":"10.1021\/acs.biomac.6c01145","type":"journal-article","created":{"date-parts":[[2026,8,6]],"date-time":"2026-08-06T15:01:44Z","timestamp":1786028504000},"page":"6143-6155","source":"Crossref","is-referenced-by-count":0,"title":["Design and Characterization\nof Self-Assembling Peptide\n(SAP)\u2013Polyethylene Glycol (PEG) Multiblock Copolymers (MBCP)\nThin Films"],"prefix":"10.1021","volume":"27","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0987-6677","authenticated-orcid":true,"given":"Nastaran","family":"Zoghi","sequence":"first","affiliation":[{"name":"The University of Manchester , , Oxford Road , ,","place":["Manchester, U.K., M13 9PL"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7437-123X","authenticated-orcid":true,"given":"Lu Shin","family":"Wong","sequence":"additional","affiliation":[{"name":"The University of Manchester , , Oxford Road , ,","place":["Manchester, U.K., M13 9PL"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mohammed","family":"Jamali","sequence":"additional","affiliation":[{"name":"The University of Manchester , , Oxford Road , ,","place":["Manchester, U.K., M13 9PL"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4958-1155","authenticated-orcid":true,"given":"Lee A.","family":"Fielding","sequence":"additional","affiliation":[{"name":"The University of Manchester , , Oxford Road , ,","place":["Manchester, U.K., M13 9PL"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Aline F.","family":"Miller","sequence":"additional","affiliation":[{"name":"The University of Manchester , , Oxford Road , ,","place":["Manchester, U.K., M13 9PL"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5504-8306","authenticated-orcid":true,"given":"Alberto","family":"Saiani","sequence":"additional","affiliation":[{"name":"The University of Manchester , , Oxford Road , ,","place":["Manchester, U.K., M13 9PL"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,6]]},"reference":[{"key":"2026091407072329000_cit1","doi-asserted-by":"publisher","first-page":"1801","DOI":"10.1038\/s41467-026-68513-1","article-title":"Mechanical forces from intercellular\npeptide self-assembly drive spheroid formation","volume":"17","author":"Lu","year":"2026","journal-title":"Nat. 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