Ultralow‐Temperature Icephobic Supramolecular Ionogels With Self‐Cleaning, Self‐Healing, Broad‐Spectrum Substrate Adhesion, and Solvent‐Triggered Recyclability

ABSTRACT Polar regions hold strategic significance for future energy exploitation and resource development, but ultralow temperatures drive severe surface icing that degrades critical equipment. Existing icephobic technologies lack the ultralow‐temperature adaptability and durability required for polar deployment. Here, a synergistic design strategy integrating supramolecular interactions with a microscale rigid–soft heterogeneous structure is developed to construct a transparent supramolecular icephobic ionogel (F_PI‐ILs@D&P). The optimized F_PI‐ILs@D&P reduces the ice adhesion strength to 6.80 kPa at −30°C (≈99.1% reduction relative to the bare substrate) and maintains < 60 kPa at −80°C. By leveraging surface‐enriched hollow cage‐like polyhedral oligomeric silsesquioxane (POSS) to confine silicone oil, the coating exhibits enhanced icephobic durability, maintaining ice adhesion below 15 kPa at −30°C after 105 icing/shear detachment cycles. The broad cryogenic icephobicity is attributed to cooperative effects of low‐modulus interfacial deformation, a confined nonfreezing ILs–H 2 O layer, POSS‐driven reduction in the ice–coating contact area, and crack propagation induced by microscale rigid–soft heterogeneity. Enabled by supramolecular interactions within the gel matrix, at gel–substrate, and gel–solvent interfaces, the coating also exhibits autonomous self‐cleaning, self‐healing, broad‐spectrum substrate adhesion, and strongly polar solvent‐triggered recyclability, effectively enhancing its environmental adaptability. This work provides a feasible strategy for developing functional icephobic surface suited to ultralow‐temperature environments.