In order to prepare flexible thermal protection aerogel materials, using dimethyldimethoxysilane (DMDMS) and methyltrimethoxysilane (MTMS) as co-precursors, isocyanate-propyltrimethoxysilane (CFS-006) was added to the co-precursor as a coupling agent, and resorcinol and formaldehyde were added to the sol solution to prepare a phenolic silicone hybrid aerogel (FAS) by the sol–gel method. The prepared FAS aerogel had no phase separation problem, the density was only 0.118 g/cm3, the hydrophobic angle reached 155.3°, and it had certain flexibility. It could be compressed to 70% and still be restored to its original state. The FAS aerogel also had a low thermal conductivity of 0.0318 W/(m·K) and good high temperature insulation. The introduction of phenolic groups improved thermal stability; Tmax increased to 643.7 °C, and the residual carbon rate was 24.5%. This work has positive significance for the future combination of aerogels and textiles in the preparation of firefighting protective clothing.