“…Supramolecular polymers consist of polymeric arrays of monomer units held together by highly directional noncovalent bonds. − Since Lehn’s pioneering work in 1990, significant efforts have been directed toward constructing various types of supramolecular polymers, driven by multiple hydrogen bonds, − host–guest complexation, − metal–ligand coordination, , and π–π stacking interactions. − The reversibility and dynamic nature of these noncovalent interactions endow supramolecular polymers with stimuli-responsiveness, holding promising prospects in applications such as self-healing, shape-memory, and recyclable materials. − External stimuli can dynamically transform supramolecular polymers in several ways, including (i) triggering the depolymerization of supramolecular polymers into monomeric species, (ii) inducing transformations between different types of supramolecular polymers, (iii) activating a “dormant” monomer, leading to in situ supramolecular polymerization, and (iv) enabling time-programmable supramolecular polymerization. To further advance the field and promote the applications of stimuli-responsive supramolecular materials, fundamental research in supramolecular polymer chemistry should focus on three key aspects: (i) designing novel types of stimuli-responsive supramolecular polymers, (ii) understanding the interplay and cooperativity of various noncovalent interactions at the molecular level, which govern self-organization and adaptivity of stimuli-responsive supramolecular polymers, and (iii) investigating the dynamics of conversion under external stimuli.…”