Artificial chlorophyll–peptide complexes were prepared by mixing ionic chlorophyll derivatives and oligopeptides in aqueous media containing a small amount of organic solvent. The pigment–peptide complexes provided chlorophyll assemblies showing a sharp red-shifted Qy absorption band concomitant with giant circular dichroism signals. The polypeptide-assisted assemblies of chlorophyllous pigments would afford a good model for photosynthetic apparatuses such as pigment–protein complexes of light-harvesting antennas.