Free-standing, stimuli-responsive polyelectrolyte multilayer films enabled by light-induced degradation of sacrificial compartments are introduced. Two examples are described: i) a triple responsive film that uses light, redox, and pH for different functions, and ii) different wavelengths of light for different functions. This approach to multiresponsive materials offers simple design and chemical synthesis while enabling different stimuli to perform separate functions in the same material.

Combining the numerous advantages of using light as a stimulus, simple free radical random copolymerization, and the easy, all-aqueous preparation of polyelectrolyte complexes (PECs), we prepared photolabile PEC nanoparticles and demonstrated their rapid degradation under UV light. As a proof of concept demonstration, the dye Nile Red was encapsulated in the PECs and successfully released into the surrounding solution as the polyelectrolyte nanocomplex carriers dissolved upon light irradiation.