Carbon nanotubes (CNTs) have been regarded as a promising material for highly sensitive gas sensors due to their excellent material properties combined with their one-dimensional structural advantages, i.e., a high surface-to-volume ratio. Here we demonstrate a CNT-based gas sensor based on assembling highly purified, solution-processed 99.9% semiconducting CNT networks bridged by palladium source/drain electrodes in a field-effect transistor (FET) configuration with a local back-gate electrode. We investigated the gas responses of the CNT-FETs under different controlled operating regimes for the enhanced detection of H2 and NO2 gases using sensors with various physical dimensions. With the aid of the CNTs with high semiconducting purity (99.9%), we achieved excellent electrical properties and gas responses in the sensors and clearly determined that the operating regimes and physical dimensions of the sensors should be appropriately adjusted for enhanced sensing performance, depending on the gas molecules to be detected.