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Herein, we report the formation of a novel, patterned cross\u2010\u03b2 structure formed by self\u2010assembled <jats:italic>C<\/jats:italic><jats:sub>3<\/jats:sub>\u2010symmetric peptide amphiphiles based on diphenylalanine and benzene\u20101,3,5\u2010tricarboxamide (BTA). The cross\u2010\u03b2 motif is an abundant structural element in amyloid fibrils and aggregates of fibril\u2010forming peptides, including diphenylalanine. The incorporation of topological constraints on one edge of the diphenylalanine fragment limits the number of \u03b2\u2010strands in \u03b2\u2010sheets and leads to the creation of an unconventional offset\u2010patterned cross\u2010\u03b2 structure consisting of short 3\u00d72 parallel \u03b2\u2010sheets stabilized by phenylalanine zippers. In the reported assembly, two patterned cross\u2010\u03b2 structures bind parallel arrays of BTA stacks in a superstructure within a single\u2010molecule\u2010thick nanoribbon. In addition to a threefold network of hydrogen bonds in the BTA stack, each molecule becomes simultaneously bound by hydrogen bonds from three \u03b2\u2010sheets and four phenylalanine zippers. The diffuse layer of alkyl chains with terminal polar groups prevents the nanoribbons from merging and stabilizes cross\u2010\u03b2\u2010structure in water. Our results provide a simple approach to the incorporation of novel patterned cross\u2010\u03b2 motifs into supramolecular superstructures and shed light on the general mechanism of \u03b2\u2010sheet formation in <jats:italic>C<\/jats:italic><jats:sub>3<\/jats:sub>\u2010symmetric peptide amphiphiles.<\/jats:p>","DOI":"10.1002\/chem.202303194","type":"journal-article","created":{"date-parts":[[2023,11,15]],"date-time":"2023-11-15T16:09:40Z","timestamp":1700064580000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["An Offset Patterned Cross\u2010\u03b2 Structure in Assemblies of <i>C<\/i><sub>3<\/sub>\u2010Symmetric Peptide Amphiphiles"],"prefix":"10.1002","volume":"30","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-0396-4353","authenticated-orcid":false,"given":"Oleksandr","family":"Zagorodko","sequence":"first","affiliation":[{"name":"Polymer Therapeutics Lab Centro de Investigaci\u00f3n Pr\u00edncipe Felipe  C\/d'Eduardo Primo Y\u00fafera, 3 46012 Valencia Spain"},{"name":"Institute for Complex Molecular Systems (ICMS) Eindhoven University of Technology  P.\u2009O. 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