Tuning Dry and Wet Adhesion with a Branched Supramolecular Polymer Solution

Endowing adhesives with both dry and wet adhesion to surfaces from hard substrates to soft biological tissues is challenging. Herein, a branched supramolecular polymer is introduced in dry‐ and wet‐crosslinking forms to adaptively achieve dry and wet interfacial adhesion. The branched supramolecular polymer (PAMU) with multiple pendant functional moieties is prepared by one‐pot reversible addition‐fragmentation chain transfer polymerization. The PAMU polymer solution can firmly adhere to glass sheets after the water evaporates. The aqueous solution of PAMU polymer with residual double bonds can be further polymerized to form a wet crosslinking network. The hydrogen bonding moieties endow the supramolecular network with self‐healing properties, while the in situ polymerization of the PAMU polymer leads to stable adhesion to wet tissues. This study provides a promising approach to develop supramolecular adhesives for versatile adhesion applications.