▎ 摘　　要

High porosity combined with mechanical durability in conductive materials is in high demand for special applications in energy storage under limiting conditions, and it is fundamentally important for establishing a relationship between the structure/chemistry of these materials and their properties. Herein, polymer-assisted self-assembly and cross-linking are combined for reduced graphene oxide (rGO)-based aerogels with reversible compressibility, high elasticity, and extreme durability. The strong interplay of crosslinked rGO (x-rGO) aerogels results in high porosity and low density due to the re-stacking inhibition and steric hinderance of the polymer chains, yet it makes mechanical durability and structural bicontinuity possible even under compressive strains because of the coupling of directional x-rGO networks with polymer viscoelasticity. The x-rGO aerogels retain >140% and >1400% increases in the gravimetric and volumetric capacitances, respectively, at 90% compressive strain, showing reversible change and stability of the volumetric capacitance under both static and dynamic compressions; this makes them applicable to energy storage devices whose volume and mass must be limited.