Achieving Intrinsically Self‐Healing Fabrics with Breathability, Surface Self‐Repairing, and Underwater Adhesion via Nanoparticle‐Polymer Gel Synergistic Coatings

Abstract Self‐healing fabrics have attracted increasing attention as a sustainable solution to extend fabric lifespan and reduce material waste. However, most reported self‐healing fabrics rely on extrinsic systems with limited healing cycles, or intrinsic polymers that compromise breathability due to irreversible layer adhesion. In this work, a simple and scalable dip‐coating method is reported to fabricate intrinsically self‐healing fabrics that retain their porous structure and air permeability. Commercial fabrics are coated with surface‐modified silica nanoparticles (SiNPs) and a polymeric ionic gel (PIG) composed of poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVDF‐HFP) and ionic liquid ([EMI] ⁺ [TFSI] ⁻ ). The SiNPs enhance coating durability and hydrophobicity, while the PIG enables intrinsic self‐healing via ion–dipole interactions. The resulting fabrics exhibit rapid and repeatable self‐healing at room temperature, even underwater, while maintaining breathability and repellency to various liquids. Furthermore, the PIG solution can be applied as a reversible adhesive or touch fastener, highlighting its multifunctionality. This study provides a versatile platform for the development of smart textiles with enhanced durability, self‐healing, and customizable adhesion properties.