Bioinspired supramolecular fibrillization enables stretchable and biodegradable piezoelectric bioelectronics.

Bioinspired piezoelectricity is extensively explored for diverse bio-machine interface and biomedical engineering applications. Nevertheless, state-of-the-art bio-piezoelectricity mainly focuses on crystallization. Yet, crystalized structures exhibit several shortcomings, including limited biocompatibility or biodegradability along with intrinsic non-stretchability. Herein, peptides fibrillization is reported to present inherent bio-piezoelectricity. Upon forming double-network framework with silk fibroin, fibrous peptide piezogels of innate biocompatibility and biodegradability are achieved, showing a programmable piezoelectricity. In particular, the bioinspired supramolecular piezogel can linearly respond to external compression and stretching in large force regions, extensively expanding the application potential bio-piezoelectricity. Upon designing a "W"-shaped structural conformation, a peptide fibrous piezogel-based piezoelectric sensor is shown to be used for detection of limb movements and subcutaneous implantation of the bioinspired piezoelectric electronics, realizing in situ and real-time monitoring of stimuli responses. The findings suggest the promising potential of peptide fibrillization-based bio-piezoelectricity for diverse bio-machine interface and biomedical engineering applications.