Efforts to obtain high-strength graphene sheets by near-room-temperature assembly have been frustrated by the misalignment of graphene layers, which degrades mechanical properties. While in-plane stretching can decrease this misalignment, it reappears when releasing the stretch. Here we use covalent and π-π inter-platelet bridging to permanently freeze stretch-induced alignment of graphene sheets, and thereby increase isotropic in-plane sheet strength to 1.55 GPa, in combination with a high Young's modulus, electrical conductivity and weight-normalized shielding efficiency. Moreover, the stretch-bridged graphene sheets are scalable and can be easily bonded together using a commercial resin without appreciably decreasing the performance, which establishes the potential for practical applications.
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