Strong Adhesives Mediated by Dynamic Phase‐Locking

Nature has long inspired the design of reversible smart adhesives; however, achieving both high adhesion strength and switchability remains a significant challenge, particularly for emerging applications (e.g., soft robotics and wearable electronics). Herein, we introduce switchable phase-locking-mediated adhesives (SPAs) that leverage high-density hydrogen bonds to deliver ultrahigh adhesion (up to 15 MPa). The underlying mechanism involves dynamic phase-locking mediation that harmonizes interfacial adhesion with bulk cohesion through interfacial mechanical locking and strain-induced phase separation. This strategy optimizes performance across the complete adhesion lifecycle, including spreading, adhering, and debonding via temperature/force-mediated phase-locking. Through detailed molecular analysis of the SPA system, we uncover the mechanistic basis of ultrahigh adhesion and establish design guidelines applicable to future smart adhesive development.