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However, the impact of stereoselective solvent\u2013solute interaction on piezoelectric performance remains poorly understood. Herein, we report a heterochiral solvent\u2013solute matching strategy for enhancing the piezoelectricity of supramolecular nanostructures assembled from enantiomeric phenylalanine derivatives, (S)-AD or (R)-AD. Piezoelectric output is strongly dependent on solvent chirality: The heterochiral (S)-CPA produces an even greater enhancement of 200% compared to homochiral solvent (R)-CPA. Time-resolved studies and molecular dynamics (MD) simulations reveal that the chiral solvent transiently engages (S)-AD at the initial assembly stage and then progressively disengages as assembly proceeds. Spectroscopic studies and density functional theory (DFT) suggest that conformation of (S)-AD undergoes a permanent change after this process, and the favorable conformation with higher molecular dipole moment is achieved via heterochiral (R)-CPA. This work establishes a heterochiral matching strategy via solvent\u2013solute chiral recognition to amplify electromechanical coupling, providing a paradigm for designing high-performance organic piezoelectrics.<\/jats:p>","DOI":"10.1021\/acsami.6c11373","type":"journal-article","created":{"date-parts":[[2026,9,10]],"date-time":"2026-09-10T23:01:25Z","timestamp":1789081285000},"page":"51397-51408","source":"Crossref","is-referenced-by-count":0,"title":["Enhanced Piezoelectric Response via Transient Heterochiral Solvent\u2013Solute Matching in Supramolecular Assembly"],"prefix":"10.1021","volume":"18","author":[{"given":"Jingyi","family":"Xia","sequence":"first","affiliation":[{"name":"Shanghai Jiao Tong University , , 800 Dongchuan Road , ,","place":["Shanghai, P. R. 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