<p>Low-dimensional materials are expected to play critical roles in next-generation electronic and optoelectronic devices, yet their controlled synthesis remains challenging. This is particularly true for emerging materials with interesting properties such as tellurium. Here we present a molecular engineering approach to synthesize wafer-scale, uniaxially oriented Te nanowire thin films with excellent controllability and uniformity. We show that molecules with an anchor-rope structure can facilitate the oriented growth of Te nanowires on m-plane sapphire. The resulting Te nanowires are well arranged, with 99.7% of them having a 5° angular spread across a 1.3-inch scale. Te nanowire thin film-based transistors show high-performance p-type characteristics. They demonstrate an average room-temperature mobility of 270 cm²V⁻¹ s⁻¹, with a maximum value reaching up to 560 cm²V⁻¹ s⁻¹, and on/off ratios as high as 10⁴. Our work lays the foundations for the application of low-dimensional tellurium, and the substrate molecule-engineering strategy may offer insights into the controlled synthesis of other low-dimensional functional materials.</p><p></p>