Graphene Nanoribbon Core Thermotropic Liquid Crystal with a Well‐Defined Molecular Structure

Abstract Graphene nanoribbons (GNRs) with hierarchical and well‐ordered structures are believed to deliver superior performance in semiconductor device applications. Despite this potential, traditional alignment techniques for GNRs often fall short in producing defect‐free and precisely defined molecular architectures. Here, we introduce a strategy for the fabrication of highly ordered GNR by empowering them with thermotropic liquid crystallinity, utilizing a bottom‐up solution synthesis approach. The resulting GNR liquid crystal ( GNR‐LC ) molecule can self‐assemble into a hexagonal columnar phase. The homeotropic alignment of GNR‐LC is enabled by the intrinsic self‐assembly capabilities of the thermotropic liquid crystalline state, thereby forming 1D charge transport pathways. Devices incorporating GNR‐LC have demonstrated significantly enhanced hole mobility, reaching up to 2.4 cm 2  V −1 s −1 , underscoring their viability as organic semiconductors for optoelectronic applications.