Supramolecular/Dynamic Covalent Design of High‐Performance Pressure‐Sensitive Adhesive from Natural Low‐Molecular‐Weight Compounds

Abstract Adhesive materials have played an essential role in the history of humanity. Natural adhesives composed of low‐molecular‐weight monomers have been overshadowed by modern petroleum‐based glues. With the development of green economy, the demand for eco‐friendly materials has increased. Herein, two natural biocompatible compounds, namely thioctic acid ( TA ) and malic acid ( MA ), are selected to prepare a high‐performance pressure‐sensitive adhesive poly[ TA ‐ MA ]. This adhesive can be quantitatively obtained via a simple mixing and heating process. Poly[ TA ‐ MA ] shows interesting and useful properties, including reversible flexibility, high elongation, and good self‐healing, owing to its dynamic polymerization pattern and reversible cross‐linking behavior. Poly[ TA ‐ MA ] exhibits excellent adhesion performance under various extreme conditions, such as at low temperatures and in hot water. High values of shear strength (3.86 MPa), peel strength (7.90 N cm −1 ), loop tack (10.60 N cm −1 ), tensile strength (1.02 MPa), and shear resistance (1628 h) demonstrate the strong adhesive effect of poly[ TA ‐ MA ]. Additionally, TA can be regenerated in the monomer forms from poly[ TA ‐ MA ] with high recovery rate (>90%). Meanwhile, strong anti‐bacterial behavior of poly[ TA‐MA ] is recorded. This study not only reported a new pressure‐sensitive adhesive but also fully displayed the feasibility of using natural small molecules to achieve robust surface adhesion.