Aerogels are lightweight materials with extensive microscale pores, which could be used in thermal insulation, energy devices, aerospace structures, as well as emerging technologies of flexible electronics. However, traditional aerogels based on ceramics tend to be brittle, which limits their performance in load-bearing structures. Due to restrictions posed by their building blocks, recently developed classes of polymeric aerogels can only achieve high mechanical strength by sacrificing their structural porosity or lightweight characteristics.