Three diacetylene macromonomers based on oligopeptide-polymer conjugates were designed to self-organize into uniform supramolecular polymers which exhibited multiple-helical superstructures constituted from a defined, finite number of laminated single beta-sheet tapes. These supramolecular polymers were then converted into poly(diacetylene)s with multiple-helical quaternary structures. The nature of the latter in solution was investigated by UV, CD, and Raman spectroscopy. The polymerization proceeded under preservation of the previously assembled multiple-helical superstructures, and the deaggregation of the oligopeptide beta-sheets before and after polymerization proved the mutual stabilization of the helical poly(diacetylene) backbone conformation and hydrogen bonded beta-sheet arrays.