Recently, tellurium (Te), a group-VI element semiconductor, has garnered considerable attention owing to its exceptional electrical properties and high stability, offering broad application potential. However, the electron conduction mechanism in Te-based semiconductor devices remains obscure owing to the unintentional p-doping caused by the native atomic vacancies present in Te materials. Herein, we report the carrier-typedependent Coulomb scattering mechanism in ambipolar Te fieldeffect transistors via high-κ dielectric passivation of Al 2 O 3 using the atomic layer deposition technique. The populated excess electrons (≈5.4 × 10 12 cm −2 ) after Al 2 O 3 deposition lead to the presence of ambipolarity, allowing simultaneous exploration of the charge scattering mechanisms of electrons and holes in an identical Te channel. The dominant charged carrier fluctuation can be attributed to variations in the number of carriers accumulated at the SiO 2 /Te and Te/Al 2 O 3 interfaces through dynamic carrier trapping and detrapping from the surrounding oxide trap sites via tunneling. The determined effective trap surface density of dielectrics for electrons (≈3.2 × 10 13 cm −2 •eV −1 ) and holes (≈3.6 × 10 13 cm −2 •eV −1 ) is approximately six to seven times lower than that of Te vacancies (≈2.1 × 10 14 cm −2 •eV −1 ), highlighting the critical role of Te vacancies in achieving ambipolar transport. In addition, we demonstrated the NOT logic gate application based on ambipolar 2D Te FETs. Our study suggests a strategy for achieving n-type doping for complementary metal−oxide−semiconductor applications and provides insights into the charge scattering mechanisms in ambipolar Te-based electronic devices.