AbstractCarbon nanotube (CNT) field effect transistors (CNFETs) show promise for the next generation VLSI systems due to their excellent scalability, energy efficiency, and speed. However, high leakage current is a drawback of large diameter CNTs (diameter (DCNT) ≥ 1.4 nm) due to the small electronic band gap (EG) ≤ 0.6 eV and effective mass. This work investigates the on‐current and off‐current tradeoff for two populations of semiconducting‐enriched CNT with DCNT ≈ 1.0 nm displaying a simultaneous 50x improvement in minimun current (IMIN) with 2.5x degradation in contact resistance compared to DCNT ≈ 1.4 nm using a Pd side‐bonded contact. A method to enhance the performance of low‐leakage CNFETs is demonstrated using sub‐monolayer self‐aligned contact doping with 0.8 nm of MoOX, which delivers a 57% reduction in contact resistance to DCNT ≈ 1.0 nm. Robustness is verified after annealing at 200 °C for 30 min and monitoring stability across 6 months post‐fabrication with no change in electrical behaviors.