Polyurethane coating has been commonly used in aerospace and construction, and enhancing anti-icing capabilities in low temperatures is crucial for preventing mechanical failures and reducing energy consumption. Utilizing a superhydrophobic surface was considered an important option to improve anti-icing performance. In this study, femtosecond laser treatment has applied to polyurethane coating on glass fiber-reinforced plastic (GFRP) to transform from hydrophilic to superhydrophobic. Results have indicated that laser treatment significantly reduced the solid–liquid contact area compared to the original surface. The non-polar groups on the surface contributed greatly to the enhancement of hydrophobicity. In comparison to the original surface, the freezing temperature of droplets on the superhydrophobic surface with improved anti-icing performance was reduced from −4.5 °C to −9.2 °C, while the freezing time was extended from 65 s to 269 s. This improvement was attributed to the reduction of solid–liquid contact area, resulting in a low heat transfer rate and a low heterogeneous nucleation rate. Additionally, the laser-treated surface exhibited excellent self-cleaning effects, along with mechanical and chemical stability.