A superflexible hydrophobic silica-based aerogel (FHSA) was prepared via a facile sol−gel process and ambient pressure drying method. The FHSA was treated at different temperatures varying from −196 to 450 °C to evaluate its thermal and mechanical performances. The evolutions of the physical property, hydrophobicity, microstructure, pore structure, and chemical structure of the FHSA with the various treatment temperatures were investigated comprehensively. The structure of the FHSA did not show an obvious change after treatment in the liquid nitrogen. The bulk density of the FHSA increased from 0.047 to 0.077 g cm −3 when the thermal treatment temperature increased from 25 to 450 °C. The specific surface area and pore volume of the FHSA increased with the treatment temperature owing to the decomposition of the organic moieties. The Fourier transform infrared spectra showed that the methyl groups in the FHSA had excellent thermostability up to 400 °C. The water contact angles of the FHSA after treatment at
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