Herein, we explore the intricate pathway complexity, focusing on the dynamic interplay between kinetic and thermodynamic states, during the supramolecular self-assembly of peptides. We uncover a multiresponsive chiroptical switching phenomenon influenced by temperature, denaturation and content of cosolvent in peptide self-assembly through pathway complexity (kinetic vs. thermodynamic state). Particularly noteworthy is the observation of chiroptical switching during the denaturation process, marking an unprecedented phenomenon in the literature. Furthermore, the variation in cosolvent contents produces notable chiroptical switching effects, emphasizing their infrequent incidence. Such chiroptical switching yields switchable piezoresponsive peptide-based nanomaterials, demonstrating the potential for dynamic control over material properties. In essence, our work pioneers the ability to control piezoresponsive behavior by transforming nanostructures from kinetic to thermodynamic states through pathway complexity. This approach provides new insights and opportunities for tailoring material properties in self-assembled systems.
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