LAUSR

Icing and frosting on transparent surfaces compromise visibility on various optical equipment and transparent infrastructures. It remains challenging to fabricate energy‐saving coatings for harvesting solar energy while maintaining high transparency. Here, transparent, photothermic, and icephobic composite surfaces composed of photothermal nanomaterials and polyelectrolytes via layer‐by‐layer assembly are designed and constructed. The positively‐charged polypyrrole nanoparticles and negatively‐charged poly(acrylic acid) are assembled as exemplary materials via electrostatic attractions. The optically transparent photothermal coatings are successfully fabricated and exhibited photothermal capabilities and light‐transmittance performance. Among the various coatings applied, the seven‐bilayer coating can increase the temperature by 35 °C under 1.9‐sun illumination, maintaining high transmittance (>60%) of visible light. With sunlight illumination at subzero temperatures (> −35 °C), the coatings show pronounced capabilities to inhibit freezing, melt accumulated frost, and decrease ice adhesion. Precisely, the icephobic surfaces remain free of frost at −35 °C as long as sunlight illumination is present; the accumulated frost melts rapidly within 300 s. The ice adhesion strength decreases to ≈0 kPa as the melted water acts as a lubricant. Furthermore, the negatively‐charged graphene oxide and positively‐charged poly(diallyldimethylammonium chloride) show their material diversity applicable in the coating fabrication.