Green synthesis of aerogels with high mechanical properties has long
remained a big challenge ever since Kistler’s report in 1931. Inspired by ant nests, we report a green method to synthesize strong, superelastic and flexible silicone aerogels. The aerogels are prepared by hydrolytic condensation of silanes with trace amounts of catalyst and surfactant (0.094 mmol mol−1) followed by drying the hydrogels at ambient pressure. The aerogels can quickly recover their original shape
after repeated compression and bending. The aerogels can be functionalized via their Si−OH or vinyl groups for specific purposes. We also extend the method for forming aerogel coatings on diverse types of materials. Our study demonstrates that green synthesis of superelastic aerogels is feasible and bioinspiration is an efficient strategy.