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.