Diacetylene macromonomers based on oligopeptide-polymer conjugates reliably organized into uniform supramolecular polymers with defined hierarchical structure, strictly controlled by the number and pattern of hydrogen bonding sites. Some of the aggregates were converted into conjugated polymers under retention of their hierarchical structure, yielding soluble poly(diacetylene)s with single-stranded, double-helical, or quadruple-helical quaternary structures.