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Herein, we report the higher-order supramolecular self-assembly of rationally designed ultrashort cationic peptidomimetics by harnessing the unique conformational preferences and enhanced molecular interactions of homologated noncanonical \u03b3- and \u03b2-hydroxy-\u03b3-amino acid residues. The intrinsic amphiphilic character of these peptidomimetics drives their self-assembly into fibrillar, viscoelastic, injectable hydrogels with distinctive conformational and supramolecular organization. Furthermore, systematic structural engineering of peptidomimetics yielded a hydrogel matrix with a more hydrated microenvironment conducive for the culture of L929 fibroblast cells. Moreover, the cationic fibrillar networks exhibited potent antibacterial activity, highlighting their potential as biocompatible antimicrobial biomaterials. This study demonstrates the importance of rational structural engineering of ultrashort peptidomimetics for the generation of functional biomaterials.<\/jats:p>","DOI":"10.1021\/acs.biomac.6c00469","type":"journal-article","created":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T13:12:45Z","timestamp":1785849165000},"page":"5239-5250","source":"Crossref","is-referenced-by-count":0,"title":["Molecular Engineering\nof Minimalistic Amphiphilic\nPeptidomimetics for the Design of Biocompatible Hydrogels with Potential\nAntibacterial Activity"],"prefix":"10.1021","volume":"27","author":[{"given":"Shubhrta","family":"Singh","sequence":"first","affiliation":[{"name":"National Institute of Pharmaceutical Education and Research (NIPER) , , S.A.S. 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Nagar , ,","place":["Mohali, India, 160062"]},{"name":"National Institute of Science Education and Research (NISER) , , ,","place":["Bhubaneswar, India, 752050"]},{"name":"Training School Complex , , Anushakti Nagar , ,","place":["Mumbai, India, 400094"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,28]]},"reference":[{"issue":"5036","key":"2026081008073808400_cit1","doi-asserted-by":"publisher","first-page":"1312","DOI":"10.1126\/science.1962191","article-title":"Molecular Self-Assembly and Nanochemistry:\nA Chemical Strategy for the Synthesis of Nanostructures","volume":"254","author":"Whitesides","year":"1991","journal-title":"Science"},{"issue":"5564","key":"2026081008073808400_cit2","doi-asserted-by":"publisher","first-page":"2418","DOI":"10.1126\/science.1070821","article-title":"Self-Assembly at All Scales","volume":"295","author":"Whitesides","year":"2002","journal-title":"Science"},{"issue":"10","key":"2026081008073808400_cit3","doi-asserted-by":"publisher","first-page":"1171","DOI":"10.1038\/nbt874","article-title":"Fabrication\nof Novel Biomaterials through Molecular Self-Assembly","volume":"21","author":"Zhang","year":"2003","journal-title":"Nat. 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