Until now, materials with high elasticity at deep cryogenic temperatures have not been observed. Previous reports indicated that graphene and carbon nanotube–based porous materials can exhibit reversible mechano-elastic behavior from liquid nitrogen temperature up to nearly a thousand degrees Celsius. Here, we report wide temperature–invariant large-strain super-elastic behavior in three-dimensionally cross-linked graphene materials that persists even to a liquid helium temperature of 4 K, a property not previously observed for any other material. To understand the mechanical properties of these graphene materials, we show by in situ experiments and modeling results that these remarkable properties are the synergetic results of the unique architecture and intrinsic elastic/flexibility properties of individual graphene sheets and the covalent junctions between the sheets that persist even at harsh temperatures. These results suggest possible applications for such materials at extremely low temperature environments such as those in outer space.