Because of the unique optical properties of gold nanomaterials, the preparation of gold nanomaterials with excellent chirality has received extensive attention. In order to develop a simple fabrication method for three-dimensional chiral Au nanostructures with a size of several hundred nanometers, chiral gold nanoparticles were developed to transfer chirality of a peptide to gold nanoparticles. In this study, the controlled synthesis of asymmetric gold nanopolyhedrons was achieved. The asymmetric gold nanopolyhedrons prepared via peptide-directed growth can exhibit strong circular dichroism (∼±50 mdeg) couplets in the visible range (500-600 nm). Also, the morphology of chiral Au nanododecahedrons-peptide particles showed distorted and asymmetric properties. In order to prove that the size and spatial structure of gold nanopolyhedrons have an influence on their chiral optical properties, Au nanotrioctahedron-peptide particles were prepared by using Au nanotrioctahedrons with different morphologies. Au nanotrioctahedron-peptide particles also exhibited circular dichromatic couplets in the visible region.