Photo‐Regulated Supramolecular Polymers: Shining Beyond Disassembly and Reassembly

Abstract Stimuli‐responsive materials, especially those that can respond to light stimuli, are highly attractive and promising for scientists working in many fields. Recently, the emerging supramolecular polymers and materials are found to be versatile and reliable in the construction of smart soft materials owing to their dynamic nature. Aiming to regulate the dynamic properties of supramolecular polymers by remote external light stimuli, previous efforts have focused on the photo‐controlled assembly/disassembly of supramolecular polymers, showing several expectable applications of light‐responsive supramolecular materials. In this progress report, the recently emerging light‐responsive supramolecular polymers are summarized which exhibit conceptually new functions and applications beyond reversible disassembly/reassembly, such as light‐regulated morphology transformation, tunable fluorescent emission, switchable self‐healing ability, muscle‐like actuation, and programmed shape memory. Remaining questions and challenges to design and construct these smart optical materials are discussed in detail based on molecular engineering strategy. Additionally, several unsolved questions for light‐regulated supramolecular polymers are given to discuss the possible opportunities of this field.