“…Aerogels are excellent ultralight solid materials with a three-dimensional (3D) interconnected porous structure, which are formed by the replacement of the liquid phase in a gel with gas phase. − The interconnected porous structure renders the aerogels with ultralow density, rich porosity, large specific surface area, and extremely low thermal conductivity, making them suitable for wide applications such as environmental protection, thermal management, energy storage, catalyst carrier, and electromagnetic metamaterial. − In the past few decades, a series of aerogels based on carbon, ceramics, and polymers have been developed. − Among them, carbon-based aerogels are most attractive for their high electrical conductivity and superior thermal and chemical stability, implying their promising applications in flexible energy storage devices and wearable electronics. , Although various carbon-based aerogels with desirable performance have been achieved from nanocarbon units, they are intrinsically brittle and prone to collapse when subjected to external stress, which limit their potential for large-scale applications . Therefore, the development of robust and elastic carbon-based aerogels is currently of great interest to meet the ever-growing demands of our society.…”