The combination of ordered macromolecular structures and well-defined responsive molecular triggers is enabling precise and amplified structural and property switching in synthetic architectures leading to useful functions. These features are reminiscent of the most sought after designs in nature, specifically the ability of superstructures to form on-demand, store information, perform actuation, and store/ release molecular payloads. Such macromolecular systems arise through the precise

more »

... nt of environmentally responsive elements within polymer chains, an ability only recently possible for synthetic systems. The drivers behind such progress are described and future possibilities for functional macromolecular superstructures discussed.