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Self‐healing polymer coatings have gained increased attention as a pathway for regenerating the inherent properties of surface following mechanical, physical or chemical damages. In most cases, the adhesion between the polymer coating layer and the substrate is driven by physical interactions. For some applications, immersing the polymer coating under water or exposing the coating to organic solvent vapors will undoubtedly lead to the coating delamination. One way to circumvent this issue is to attach the coating to the substrate via covalent bonds. However, this process will impede the self‐healing feature of the polymer coating due to the confinement of the volume change of the polymer to one dimension. Herein, surface‐attached metallo‐supramolecular polymer conetwork coatings are reported. The ability of the polymer conetworks to swell in organic solvent while maintaining their dimensional stability combined with reversible supramolecular cross‐links based on metal complexes enables the design of scratch‐healing polymer coatings. These metallo‐supramolecular polymer conetworks are prepared in a three‐step UV‐initiated polymerization reaction starting from the poly(pentafluorophenyl acrylate)‐l‐polydimethylsiloxane (PPFPA‐l‐PDMS)‐activated ester covalently attached to the substrate. Reacting the polymer conetwork coating with the 4‐(2‐aminoethyl)pyridine and cross‐linking the pyridine phases with ZnCl2 lead to the poly(N‐(2(pyridin‐4‐yl)ethyl)acrylamide‐Zn(II))‐l‐polydimethylsiloxane (PNP4EA‐Zn(II)‐l‐PDMS) polymer conetwork coatings with scratch‐healing ability. [ABSTRACT FROM AUTHOR]

The current challenge in self‐healing materials resides in the design of materials which exhibit improved mechanical properties and self‐healing ability. The design of phase‐separated nanostructures combining hard and soft phases represents an attractive approach to overcome this limitation. Amphiphilic polymer conetworks are nanostructured materials with robust mechanical properties, which can be tailored by tuning the polymer composition and chemical functionality. This article highlights the design of phase‐separated nanostructured polymers from metallo‐supramolecular amphiphilic polymer conetworks, and their application for self‐healing surfaces. The synthesis of poly(N‐(pyridin‐4‐yl)acrylamide)‐l‐polydimethylsiloxane polymer conetworks from the poly(pentafluorophenyl acrylate)‐l‐polydimethylsiloxane activated ester is presented. Loading of ZnCl2 salt into the phase‐separated polymer conetwork strengthens the network by cross‐linking the poly(N‐(pyridin‐4‐yl)acrylamide) phases, while offering reversible interactions needed for self‐healing ability. [ABSTRACT FROM AUTHOR]