A cyclic dipeptide cyclo [–L-methionyl–L-methionyl–] and gold (I) cation were found to form a complex in a 1: 2 ratio. Pouring a DMF solution of the complex into ethyl acetate afforded fibers with lengths of more than 20 µm and 100–400 nm in width, which consisted of fibrous nanostructures 50–100 nm in diameter. Treatment of this supramolecular fiber with catechol gave linearly aligned Au nanoparticles on the original fibers.