Superior Hard yet Flexible, Highly Transparent, and Scratch‐Repairable Waterborne Antiadhesive Coatings Enabled by Multi‐Magnitude Dynamic Bonds Synergy Strategy

Abstract With the advent and proliferation of foldable displays, the demand for hard yet flexible antiadhesive coatings with healability has significantly increased. Unfortunately, reports on such materials are scarce, with existing research generally facing the challenge of reconciling the “trade‐off” effect among hardness, flexibility, and dynamic performance and containing high levels of volatile organic compounds which causes irreversible environmental damage. Herein, this study presents a waterborne antiadhesive coating with ceramic‐like hardness, polymer‐like flexibility, and healability. The coating is fabricated through a multi‐magnitude dynamic bond synergy strategy, wherein the synthesized amino‐rich oligosiloxane with polydimethylsiloxane (PDMS) chains is dynamically linked with the amino‐rich oligosiloxane containing ureidopyrimidinone moieties via coordination reaction between aluminum chloride hexahydrate (AlCl 3 ·6H 2 O) and amino, enabling the coating comprising Al─N coordination bonds and hierarchical hydrogen bonds. The as‐prepared coating exhibits 99.95% self‐healing efficiency while possessing superior hardness (9H), flexibility (2 mm bending radius), and transparency (>99% transmittance). In addition, the incorporation of PDMS endows the coating with excellent antiadhesive properties. More importantly, the coating formulation is entirely waterborne, aligning with environmentally sustainable practices. This research offers valuable insight for advancing the development of waterborne coatings with well‐balanced comprehensive performance, particularly suited for applications in foldable displays and other fields.