Solution-sheared supramolecular oligomers with enhanced thermal resistance in interfacial adhesion and bulk cohesion.

Developing strong, thermally resistant adhesives for load-bearing applications remains challenging. Here we report a class of solution-sheared supramolecular oligomers that exhibit exceptional adhesive strength and toughness across a broad temperature range. These adhesives achieve a debonding work up to 23.6 kN/m and a lap shear strength exceeding 30.6 MPa, surpassing commercial structural adhesives by up to eightfold on metal and glass surfaces. Impressively, they retain a lap shear strength above 21 MPa even at 120 °C, outperforming current leading commercial alternatives. This performance arises from hierarchical nanostructures formed during solution shearing, which create enlarged, ordered nanocrystals and aligned nanofibrils within the bulk, enhancing mechanical robustness and toughness. Simultaneously, hydrogen-bonded nanocrystals anchored at the surface significantly strengthen interfacial adhesion. This multiscale structural organization enables thermal tolerance, crack resistance, and efficient energy dissipation, setting a new paradigm for high-performance, reusable adhesives capable of multiple rebonding cycles. Our work demonstrates how solution-shearing simultaneously optimizes adhesion chemistry and multiscale nano/microstructural control, achieving synergistic improvements in interfacial adhesion and bulk cohesion.