Sensitized Disequilibration of Water‐Soluble Azopolymers

Abstract Photo‐responsive systems based on azobenzenes usually require UV light for E → Z isomerization, limiting their applicability, especially in biomedical contexts. Disequilibration by sensitization of azobenzene under confinement (DESC) has recently emerged as a supramolecular strategy to bypass this limitation without the need to derivatize the azobenzene scaffold. Here, we expand DESC to water‐soluble azopolymers obtained by RAFT polymerization and systematically investigate the interplay between the polymer structure and DESC efficiency. Using this approach, we achieved as much as 85% of the direct photoexcitation (UV) switching efficiency, while utilizing low‐energy (yellow) light. These results establish general design principles for combining DESC with polymeric systems, opening new opportunities for the development of functional materials driven with low‐energy light.