, which was one of the highest predicted values among peptide-based self-assemblies. The GSH assembly-based piezoelectric nanogenerator generated an open-circuit voltage of 5.02 V under an external force of 45 N, while maintaining stability over 6000 continuous press-release cycles. Furthermore, the GSH crystal-based self-powered sensor was successfully developed for effective monitoring of human joint bending. This study developed a novel natural tripeptide piezoelectric self-assembly, promoting the advancement of biomolecule-based piezoelectric supramolecular materials.