Continuous crystalline graphene papers with gigapascal strength by intercalation modulated plasticization

Graphene has an extremely high in-plane strength yet considerable out-of-plane softness. High crystalline order of graphene assemblies is desired to utilize their in-plane properties, however, challenged by the easy formation of chaotic wrinkles for the intrinsic softness. Here, we find an intercalation modulated plasticization phenomenon, present a continuous plasticization stretching method to regulate spontaneous wrinkles of graphene sheets into crystalline orders, and fabricate continuous graphene papers with a high Hermans’ order of 0.93. The crystalline graphene paper exhibits superior mechanical (tensile strength of 1.1 GPa, stiffness of 62.8 GPa) and conductive properties (electrical conductivity of 1.1 × 10⁵ S m⁻¹, thermal conductivity of 109.11 W m⁻¹ K⁻¹). We extend the ultrastrong graphene papers to the realistic laminated composites and achieve high strength combining with attractive conductive and electromagnetic shielding performance. The intercalation modulated plasticity is revealed as a vital state of graphene assemblies, contributing to their industrial processing as metals and plastics.