Ultrathin, lightweight, high‐strength, and thermally conductive electromagnetic interference (EMI) shielding materials with high shielding effectiveness (SE) are highly desired for next‐generation portable and wearable electronics. Pristine graphene (PG) has a great potential to meet all the above requirements, but the poor processability of PG nanosheets hinders its applications. Here, efficient synthesis of highly aligned laminated PG films and nacre‐like PG / polymer composites with a superhigh PG loading up to 90 wt% by a scanning centrifugal casting method is reported . Due to the PG‐nanosheets‐alignment‐induced high electrical conductivity and multiple internal reflections, such films show superhigh EMI SE comparable to the reported best synthetic material, MXene films, at an ultralow thickness. An EMI SE of 93 dB is obtained for the PG film at a thickness of ≈100 μm, and 63 dB is achieved for the PG / polyimide composite film at a thickness of ≈60 μm. Furthermore, s uch PG‐nanosheets‐based films show much higher mechanical strength (up to 145 MPa) and thermal conductivity (up to 190 W m−1 K−1) than those of their MXene counterparts. These excellent comprehensive properties, along with ease of mass production, pave the way for practical applications of PG nanosheets in EMI shielding.
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