The production of high-quality semiconducting nanostructures with optimized electrical, optical, and electromechanical properties is important for the advancement of next-generation technologies. In this context, we herein report on highly obliquely aligned single-crystalline zinc oxide nanosheets (ZnO NSs) grown via the vapor–liquid–solid approach using r-plane (01–12) sapphire as the template surface. The high structural and optical quality of as-grown ZnO NSs has been confirmed using high-resolution transmission electron microscopy and temperature-dependent photoluminescence, respectively. To assess the potential of our NSs as effective building materials in high-performance flexible electronics, we fabricate organic (parylene C)/inorganic (ZnO NS) hybrid field-effect transistor (FET) devices on flexible substrates using room-temperature assembly processes. Extraction of key FET performance …