The sophisticated use of self-organizing materials, which include liquid crystals, block copolymers, hydrogen-and pi-bonded complexes, and many natural polymers, may hold the key to developing new structures and devices in many advanced technology industries. Synthetic materials are usually designed with only one structure-forming process in mind. However, combination of both complementary and antagonistic interactions in macromolecular systems can create order in materials over many length scales. Here polymer materials that make use of competing molecular interactions are summarized, and the prospects for the further development of such materials through both synthetic and processing pathways are highlighted.