Switchable Supramolecular Adhesive by Tuning Interfacial Bonding and Modulus

ABSTRACT High‐strength and reusable adhesives are essential for many applications but are often limited by the trade‐off between strength and detachability, as well as recyclability. Here, we introduce a high‐strength supramolecular adhesive with adhesion strengths exceeding 1 MPa (up to 4.65 MPa) and remarkable detachability, achieving a switchability ratio of up to 1800. These outstanding performances are enabled by synergistically tuning interfacial physical bonds and bulk modulus of a hydrogen‐bond‐and‐dipole‐dipole‐enriched polymer (HyDiP). In its dehydrated state, the adhesive exhibits high modulus (445 MPa) and exposes rich surface bonding groups, yielding robust adhesion on various surfaces. In its rehydrated state, the modulus decreases to 0.11 MPa and the physical bond density on the surface is significantly reduced, allowing easy detachment. Furthermore, the HyDiP adhesive is transparent when dehydrated, recyclable and removable, ideal for sustainable applications like adaptive grippers and superglue for heavy loads.