Succulent‐Inspired Ultraflexible and Multifunctional Carbon Aerogel for High‐Performing Strain Sensing and Thermal Management

Abstract Porous carbon materials have exhibited many superior characteristics with extensive applications. To adequately exert their advantages at macroscale, the mechanical property plays a critical role to ensure the structural stability and functionality. Porous carbon monoliths overcome brittleness by endowing compressive superelasticity but are still plagued by poor toughness, easily suffering from the tensile, bending, or torsional fracture. Here, inspired by the biostructure of succulent plants, graphene aerogel is used to mimic the hydrenchyma tissue, carbon nanotube aerogel film as the epidermis, and graphene oxide ethanol solution as the hemicellulose binder to make ultraflexible carbon aerogels (UCAGs), addressing the critical and bottleneck issue between mechanics and functionality. The UCAGs feature a sequence of robust mechanical properties simultaneously, including compressive strain up to 99.5%, tensile strength up to 460 kPa, bending and torsional angle up to 180°. This ultraflexible aerogel is exploited for large‐deformable, and high‐sensitive strain sensor with extended working temperature (−196 to 400 °C), as well as lightweight thermal regulator with record‐high switch ratio (500:1). The high‐performance structures of this type establish a set of fundamental considerations in structural design of inorganic aerogels for a wide spectrum of applications.