<p>Chiral nanostructured Ag films (CNAFs) with lattice distorted nanoflakes were fabricated utilizing phenylalanine (Phe) as the symmetry-breaking agent and AgNO₃ as a silver source through an electrodeposition method. With prolonged electrodeposition duration or reduced applied potentials, the nanoflakes gradually thickened and enlarged, ultimately transforming into nanoblock architectures in CNAFs. The morphology of CNAFs underwent a progressive transition from nanoblocks to nanoflakes as the Phe and AgNO₃ concentrations increased. The CNAFs stacked with vertically aligned Ag nanoflakes exhibited plasmon resonance absorption-based and scattering-based optical activities in the range of 200–800 nm. It is speculated that the carboxyl and amine groups of Phe could interact with silver ions through electrostatic and coordination interactions, while the <i>π</i>-<i>π</i> stacking of Phe would facilitate the formation of chiral assemblies to achieve chirality transfer.</p>