▎ 摘　　要

The recently emergent laser-induced graphene (LIG) technology has endowed the fabrication of smart devices with one-step processing and scalable/designable features. Graphene paper (GP), an important architecture of 2D layered carbon, however, is never produced through LIG. Herein, a novel strategy is reported for production of freestanding GP through LIG technology. It is first determined that the unique spatial configuration of polyimide (PI) paper is critical for the preparation of GP without the appearance of intense shape distortion. Benefiting from the mechanism, the as-produced laser-induced graphene paper (LIGP) is foldable, trimmable, and integratable to customized shapes and structures with the largest dimension of 40 x 35 cm(2). Based on the processing-structure-property relationship study, one is capable of controlling and tuning various physical and chemical properties of LIGPs, rendering them unique for assembling flexible electronics and smart structures, e.g., human/robotic motion detectors, liquid sensors, water-oil separators, antibacterial media, and flame retardant/deicing/self-sensing composites. With the key findings, the escalation of LIGP for commercialization, roll-to-roll manufacturing, and multidisciplinary applications are highly expected.