Abstract The rapid and facile synthesis of hot melt super glue (HMSG) via the formation of adhesive supramolecular networks between catechol or pyrogallol hydroxyl groups (−OH) of polyphenols and repeat units (−CH2CH2O−) of poly(ethylene glycol) (PEG) based on hydrogen bonds is reported. The adhesion strength of HMSG, processed by heating–cooling of polyphenols and PEG without additional solvents, can be tuned up to 8.8 MPa via changing the molecular weight of PEG and the ratio of hydrogen bonding donors and receptors. The advantages of the reported HMSG lie in the ease and scalability of the assembly process, rapid adhesion on various substrates with excellent processability, resistance of low temperature and organic solvents, and recyclable adhesion strength. The solvent‐free HMSG represents a promising adhesive supramolecular network to expand the versatility and application of polyphenol‐based materials.
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