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 GNRs 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 one-dimensional charge transport pathways. Devices incorporating GNR-LC have demonstrated significantly enhanced hole mobility, reaching up to 2.4 cm2 V-1 s-1, underscoring their viability as organic semiconductors for optoelectronic applications.