Delamination
of coating layer from polymer substrate limits the lifetime and functionality
of the protective films. Silicone coating is especially vulnerable
to photo irradiation, hydrothermal degradation, and mechanical deformation
due to the low interfacial adhesion and mechanical robustness. Herein,
an ingenious approach is developed to fabricate ultrastable and durable
silicone coating on polycarbonate (PC) substrate through well-controlled
nanoscale interfacial engineering. A nanopillar array is fabricated
on the PC surface by vacuum-assisted hot embossing using anodic aluminum
oxide (AAO) templates. Significant improvement in interfacial shear
strength (ISS) is achieved for the silicone coating on the nanostructured
PC surface. The delamination mechanism can be controlled by tuning
the nanopillar size, and the maximum ISS of 9.9 MPa was reached on
a surface with a nanopillar diameter of 320 nm. Attributed to the
increased interfacial area and mechanical interlocking structure,
the nanostructured interface can effectively dissipate interfacial
stress and prevent cracking; therefore, maintaining excellent transparency
and performance in the harsh environment. The coating exhibits extraordinary
stability and durability when subjected to UV irradiation for 168
h, hydrothermal aging for 120 h, mechanical bending for 1000 cycles,
and even surface damage. Thus, the tough silicone coating on polymer
substrate realized by nanoscale interfacial engineering is a
promising technique for highly stable and durable transparent surface
protection.