High‐Strength Plus Reversible Supramolecular Adhesives Achieved by Regulating Intermolecular Pt^II⋅⋅⋅Pt^II Interactions

Abstract Surface adhesion has a great contradiction in high strength and good reversibility given their mutually exclusive requirements of fixed crosslinked networks and dynamic chain motion. Herein, we demonstrate a supramolecular organoplatinum(II) adhesive system regulated by intermolecular Pt II ⋅⋅⋅Pt II interactions that can simultaneously achieve high‐strength and excellent reversible adhesion to various substrates. Upon alternating temperature, the assembly of suitably substituted organoplatinum(II) molecules can switch between well‐ordered and disordered states via tuning Pt II ⋅⋅⋅Pt II interactions, resulting in stable reversible adhesion even after 100 cycles with a robust strength of ≈1.25 MPa and a large on‐off ratio of ≈25. Along with the switch of Pt II ⋅⋅⋅Pt II contacts, the surface adhesion of organoplatinum(II) adhesives can be monitored by their changes in electrical signals. This study will open up new inspirations for developing high‐performance reversible adhesives.