Chiral plasmonic nanostructure draws great attention due to its unpre-cedented optical properties. However, fabricating chiral nanostructure remains challenging as the structure has to be controlled asymme-trically in three dimensions. Nature has developed an exquisite ability to create asymmetric structures using chirality transfer between organic-inorganic materials. By exploiting chirality transfer and crystallo-graphic control of materials, here, we developed novel chiral gold nanostructures with gigantic optical activity (dissymmetry factor ~ 0.2 at 622 nm). The key factor for chiral fabrication is the formation of chiral high-Miller-index surfaces and their enantioselective interaction with peptide additive molecule. Modulation of these two components allow us to achieve diverse optically active chiral structures controlled in nanometer scale. The strong optical activity at visible range was substantiated by transmission of color of particle solution under polarized light.