Molecular Engineered Crown‐Ether‐Protein with Strong Adhesion over a Wide Temperature Range from −196 to 200 °C

Abstract The inherently tenuous adhesion strength and limited environmental tolerance of supramolecular adhesives severely restrict their application scenarios. It is challenging for the development of robust adhesives with extreme temperature tolerance. Herein, we report a new type of temperature‐resistant crown‐ether‐protein (CEP) adhesive by harnessing synergistic host–guest molecular interactions between engineered crown ether and protein building blocks. The outputs of CEP adhesive demonstrate ultrahigh shearing adhesion strength of ≈22 MPa over a wide temperature range from −196 to 200 °C, superior to other established supramolecular or polymeric adhesives. The temperature‐induced phase transition and internal bound water stabilized the system and led to superb adhesion under extreme conditions. Thus, this work pioneers a molecular engineering approach for the generation of adhesives with tailored applications in extreme settings.