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Generating strong adhesion by engineered proteins has the potential for high technical applications. Current studies of adhesive proteins are primarily limited to marine organisms, e.g., mussel adhesive proteins. Here, we present a modular engineering strategy to generate a type of exotic protein adhesives with super strong adhesion behaviors. In the protein complexes, the lanmodulin (LanM) underwent α‐helical conformational transition induced by lanthanides, thereby enhancing the stacking density and molecular interactions of adhesive protein. The resulting adhesives exhibited outstanding lap‐shear strength of ≈31.7 MPa, surpassing many supramolecular and polymer adhesives. The extreme temperature (−196 to 200 °C) resistance capacity and underwater adhesion performance can significantly broaden their practical application scenarios. Ex vivo and in vivo experiments further demonstrated the persistent adhesion performance for surgical sealing and healing applications. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]