A novel natural drying (ND) strategy for low-cost and simple fabrication of graphene aerogels (GAs) is highlighted. The as-formed NDGAs exhibit ultralarge reversible compressibility (99%) and tunable Poisson's ratio behaviors (-0.30 < nu < 0.46), which suggests promising applications in soft actuators, soft robots, sensors, deformable electronic devices, drug release, thermal insulator, and protective materials.