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Herein, the first integrated supramolecular investigation of pepsin\u2010digested gliadin peptides (p\u2010gliadin) is presented in combination with its functional behavior in the Caco\u20102 cell line.<\/jats:p><\/jats:sec><jats:sec><jats:title>Methods and Results<\/jats:title><jats:p>First, gliadins are degraded by pepsin at pH 3, and the physicochemical properties of p\u2010gliadin are compared with gliadin. An integrated approach using interfacial, spectroscopic, and microscopic techniques reveals that the p\u2010gliadin forms spontaneously soluble large supramolecular structures, mainly oligomers and fibrils, capable of binding amyloid\u2010sensitive dyes. The self\u2010assembly of p\u2010gliadin starts at a concentration of 0.40 \u00b5g mL<jats:sup>\u22121<\/jats:sup>. Second, the stimulation of Caco\u20102 cells with the p\u2010gliadin supramolecular system is performed, and the mRNA expression levels of a panel of genes are tested. The experiments show that p\u2010gliadin composed of supramolecular structures triggers significant mRNA up\u2010regulation (p &lt; 0.05) of pro\u2010apoptotic biomarkers (ratio Bcl2\/Bak\u20101), chemokines (CCL2, CCL3, CCL4, CCL5, CXCL8), and the chemokine receptor CXCR3.<\/jats:p><\/jats:sec><jats:sec><jats:title>Conclusions<\/jats:title><jats:p>This work demonstrates that p\u2010gliadin is interfacial active, forming spontaneously amyloid\u2010type structures that trigger genes in the Caco\u20102 cell line involved in recruiting specialized immune cells.<\/jats:p><\/jats:sec>","DOI":"10.1002\/mnfr.202100200","type":"journal-article","created":{"date-parts":[[2021,6,10]],"date-time":"2021-06-10T19:22:11Z","timestamp":1623352931000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":18,"title":["Pepsin Digest of Gliadin Forms Spontaneously Amyloid\u2010Like Nanostructures Influencing the Expression of Selected Pro\u2010Inflammatory, Chemoattractant, and Apoptotic Genes in Caco\u20102 Cells: Implications for Gluten\u2010Related Disorders"],"prefix":"10.1002","volume":"65","author":[{"given":"Maria Georgina","family":"Herrera","sequence":"first","affiliation":[{"name":"Department of Chemistry Organic Chemistry III Bielefeld University  Universit\u00e4tsstr. 25 Bielefeld 33615 Germany"},{"name":"Institute of Biological Chemistry and Physical Chemistry Dr. Alejandro Paladini, University of Buenos Aires\u2010CONICET  Buenos Aires C1113AAD Argentina"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Francesco","family":"Nicoletti","sequence":"additional","affiliation":[{"name":"Department of Chemistry Organic Chemistry III Bielefeld University  Universit\u00e4tsstr. 25 Bielefeld 33615 Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6780-2532","authenticated-orcid":false,"given":"Marion","family":"Gras","sequence":"additional","affiliation":[{"name":"Department of Chemistry Organic Chemistry III Bielefeld University  Universit\u00e4tsstr. 25 Bielefeld 33615 Germany"},{"name":"Department of Chemistry Physical and Biophysical Chemistry Bielefeld University  Universit\u00e4tsstr. 25 Bielefeld 33615 Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Philipp W.","family":"D\u00f6rfler","sequence":"additional","affiliation":[{"name":"Department of Chemistry Organic Chemistry III Bielefeld University  Universit\u00e4tsstr. 25 Bielefeld 33615 Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nicolo","family":"Tonali","sequence":"additional","affiliation":[{"name":"Department of Chemistry Organic Chemistry III Bielefeld University  Universit\u00e4tsstr. 25 Bielefeld 33615 Germany"},{"name":"Facult\u00e9 de Pharmacie, Universit\u00e9 Paris\u2010Saclay  BioCIS, 5 rue Jean\u2010Baptiste Cl\u00e9ment Ch\u00e2tenay\u2010Malabry 92296 France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yvonne","family":"Hannappel","sequence":"additional","affiliation":[{"name":"Department of Chemistry Physical and Biophysical Chemistry Bielefeld University  Universit\u00e4tsstr. 25 Bielefeld 33615 Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Inga","family":"Ennen","sequence":"additional","affiliation":[{"name":"Department of Physics Bielefeld University  Universit\u00e4tsstr. 25 Bielefeld 33615 Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Andreas","family":"H\u00fctten","sequence":"additional","affiliation":[{"name":"Department of Physics Bielefeld University  Universit\u00e4tsstr. 25 Bielefeld 33615 Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Thomas","family":"Hellweg","sequence":"additional","affiliation":[{"name":"Department of Chemistry Physical and Biophysical Chemistry Bielefeld University  Universit\u00e4tsstr. 25 Bielefeld 33615 Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Karen M.","family":"Lammers","sequence":"additional","affiliation":[{"name":"Department of Chemistry Organic Chemistry III Bielefeld University  Universit\u00e4tsstr. 25 Bielefeld 33615 Germany"},{"name":"Tubascan Ltd.  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