▎ 摘　　要

Large-area bulk oxidized cellulose nanocrystal (OCNC)/graphene nanocomposites with highly oriented structures were produced through a straightforward, cost-effective large-scale evaporation-induced self-assembly process followed by thermal curing. Well-aligned nano-sized graphene layers were evident and separated by the OCNC planar layers, which facilitate highly interconnected and continuous thermal transport parallel to the alignment. Hence, the laminated graphene-based nanocomposites possess an excellent in-plane thermal conductivity of 25.66 W/m K and a thermal conductivity enhancement (eta) of 7235% with only a 4.1 vol % graphene loading. This value is the highest recorded among all laminated composite films with <70 wt % filler content reported to date. Using this design strategy, other large-area aligned composites with other functional nanomaterials, already in large-scale production, can be made for use in a wide range of applications.