The low on-current and direct source-to-drain tunneling (DSDT) issues are the main drawbacks in the ultrascaled tunneling field-effect transistors based on carbon nanotube and ribbons. In this article, the performance of nanoscale junctionless carbon nanotube tunneling field-effect transistors (JL CNTTFETs) is greatly improved by using the synergy of electrostatic and chemical doping engineering. The computational investigation is conducted via a quantum simulation approach, which solves self-consistently the Poisson equation and the non-equilibrium Green’s function (NEGF) formalism in the ballistic limit. The proposed high-performance JL CNTTFET is endowed with a particular doping approach in the aim of shrinking the band-to-band tunneling (BTBT) window and dilating the direct source-to-drain tunneling window, while keeping the junctionless paradigm. The obtained improvements include the on-current, off-current, ambipolar behavior, leakage current, I60 metric, subthreshold swing, current ratio, intrinsic delay, and power-delay product. The scaling capability of the proposed design was also assessed, where greatly improved switching performance and sub-thermionic subthreshold swing were recorded by using JL CNTTFET with 5 nm gate length. Moreover, a ferroelectric-based gating approach was employed for more enhancements, where further improvements in terms of switching performance were recorded. The obtained results and the conducted quantum transport analyses indicate that the proposed improvement approach can be followed to improve similar cutting-edge ultrascaled junctionless tunnel field-effect transistors based on emerging atomically thin nanomaterials.