Peptides self-assembling nanoarchitectures have been found to show intrinsic piezoelectricity, thus presenting promising potentials for diverse advanced applications. Herein, we would like to introduce our recent progress on peptides architectonical piezoelectricity, focusing on the molecular mechanisms underlying piezoelectric peptide crystallization, fabrication & application of large-scale peptide crystals-arraying piezoelectricity and peptides hydrogelation piezoelectricity. Our findings suggest that the architectonical piezoelectricity may bear inspiring implications on facilitating peptides self-assembly for contributing in human lives.