Photothermal-Responsive Carbon Architectures Synergized with Multiscale Hybrid Fibers Endow Silicone Rubber with Adaptive Deformation and Survivability under Severe Scouring Thermal Conditions

Intelligent thermal protection materials were developed by incorporating molecularly intercalated graphite intercalation compounds (GICs) as functional units. The temperature-responsive performance of GICs was optimized via orthogonal experimental design (L9(33)), achieving a 500% expansion ratio at 500 °C in silicone rubber composites. Mussel-inspired polydopamine (PDA) functionalization endowed dual-stimuli responsiveness (808 nm NIR activation and thermal activation) while enhancing thermal stability through radical scavenging. Multiscale fiber hybridization with millimeter-scale carbon fibers (3 mm) and carbon nanotubes (3–12 μm) created a fence-like architecture with 59.1% porosity, maintaining >50% expansion across 200–500 °C. This hierarchical structure reduced the mass ablation rate to 0.039 g/s and demonstrated exceptional thermal insulation, limiting back-face temperatures to 179 °C under extreme conditions (0.7 MPa gas pressure, surface temperatures >1800 °C). The surface-dense/internal-porous gradient design synergized adaptive sealing with ablation resistance, offering a novel strategy for stimulus-responsive materials in extreme environments.