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Among functional biomaterials, piezoelectric materials are particularly valuable for developing self\u2010powered biodevices in biomedical applications. However, peptide\u2010based piezoresponsive systems remain largely underexplored. In this study, we present a chromophore\u2010conjugated peptide (PEP\u2010A) that self\u2010assembles into nanomaterials exhibiting either piezo\u2010active or inactive states, with the functional behaviour closely linked to their chiroptical properties under different solvent conditions. Through a comprehensive investigation involving spectroscopy, microscopy, and atomistic simulations, we uncover how cosolvent\u2010induced modulation of the self\u2010assembly process co\u2010governs chiroptical and piezoelectric properties. Interestingly, PEP\u2010A forms elongated nanofibers in pure water that are both chiroptically and piezoelectrically inactive. However, the introduction of a minimal amount of cosolvent (1% DMSO or 1% DMF) triggers the emergence of supramolecular chirality alongside a significant piezoresponse, revealing a direct correlation between macroscopic chirality and piezoelectric functionality. Our findings highlight how subtle changes in the assembly environment can drive profound shifts in material properties, offering a powerful strategy to design responsive piezoelectric biomaterials. This study provides a novel approach to designing next\u2010generation, responsive, peptide\u2010based piezoelectric biomaterials for biomedical and bioelectronic applications.<\/jats:p>","DOI":"10.1002\/anie.3135255","type":"journal-article","created":{"date-parts":[[2026,6,9]],"date-time":"2026-06-09T11:34:38Z","timestamp":1781004878000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Cosolvent\u2010Modulated Supramolecular Chirality Unveils Pronounced Piezoelectric Response in Peptide\u2010Based Nanomaterials"],"prefix":"10.1002","volume":"65","author":[{"given":"Aparna","family":"Ramesh","sequence":"first","affiliation":[{"name":"Centre For Nano and Soft Matter Sciences (CeNS)  Bengaluru India"},{"name":"Academy of Scientific and Innovation Research (AcSIR)  Ghaziabad 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