Organic Solvent‐Regulated Supramolecular Adhesives with Robust yet Reversible Adhesion

Reversible adhesives are crucial for enabling high-strength, eco-friendly bonding with on-demand detachment, yet achieving fully sustainable adhesives with high-strength and reliable detachment remains a challenge. Here, a supramolecular adhesive derived from natural materials is presented, namely, a supramolecular adhesive tailored by organic solvents (SATO), comprising tannic acid, β-cyclodextrin, and organic solvents (DMSO, ethylene glycol, or glycerol) integrated through dynamic hydrogen-bond networks. The optimized SATO achieves robust interfacial adhesion strength up to 4.1 MPa, with retained adhesion (≈0.8 MPa) even after 30 repeated bonding-debonding cycles. The adhesive demonstrates humidity-sensitive adhesion and exceptional freeze resistance, retaining ≈96% of its initial adhesion strength after 7 days of storage at -50 °C. When used to fabricate sand columns, SATO achieves compressive strengths of >11 MPa while enabling rapid on-demand disintegration within 2 s via water exposure. By synergizing eco-friendliness, high mechanical performance, and reversible adhesion, SATO holds promise for applications in arid environments and temporary structural engineering.