Superelastic and Ultralight Aerogel Assembled from Hemp Microfibers

Abstract Aerogels with both high elastic strain and fast shape recovery after compression have broad application potentials as thermal regulation, absorbents, and electrical devices. However, creating such aerogels from cellulosic materials requires complicated preparation processes. Herein, a simple strategy for scalable production of hemp microfibers using a top‐down method is reported, which can further be assembled into aerogels with interconnected porous structures via ice‐templating technique. With density as low as 2.1 mg cm −3 , these aerogels demonstrate isotropic superelasticity, as exhibited by their fast shape restoration from over 80% compressive strain. Due to the high porosity (99.87%) and structural tortuosity, these aerogels show a low thermal conductivity of 0.0215 ± 0.0002 W m −1 K −1 , suggesting their potential in thermal insulation application. Certain hydrophobic modification using silane derivative further endows these aerogels with reduced water affinity. Overall, the proposed strategy to prepare bio‐based microfibers using scalable technology, as well as the assembled aerogels, provides new insights into the design and fabrication of multifunctional bio‐based aerogels for value‐added applications.