Dual‐Terminal Molecular Strategy for Robust and Reversible Supramolecular Adhesion

Achieving strong yet reversible adhesion via minimalist molecular design remains a critical challenge for next-generation supramolecular materials. Here, a dual-end modular adhesion strategy is presented based on a small organic molecule incorporating carboxylic acid and triphenylphosphonium terminals linked by a flexible alkyl spacer. This design enables synergistic noncovalent interactions-including hydrogen bonding, dipole-dipole interactions, and electrostatic forces-to construct a thermally reconfigurable supramolecular network. Upon mild heating, the system transitions from ordered to amorphous states, facilitating dynamic cohesion and interfacial adaptability across both hydrophilic and hydrophobic substrates. The resulting adhesive achieves high lap-shear strength (up to 4.6 MPa on polyethylene terephthalate (PET)), rapid curing, and exceptional resistance to solvents, humidity, and low temperatures. Moreover, it enables fully reversible adhesion and closed-loop recyclability. Combined experimental characterizations and molecular simulations reveal how the interplay of molecular architecture and noncovalent synergy governs adhesion performance. This work provides a generalizable framework for the design of sustainable, programmable supramolecular adhesives.