Ta-based high-κ dielectrics can be synthesized via the oxidation of TaS2 films. In this study, we investigated the wet and dry oxidation of TaS2 films via thermal annealing and plasma irradiation, respectively. The specific vibration observed via Raman spectroscopy, the bonding states observed via X-ray photoelectron spectroscopy, and capacitance measurements confirmed the oxidation of TaS2 films with a dielectric constant of ~ 14.9. Moreover, the electrical transport of the TaS2 films along the in-plane direction indicated a change in conductivity before and after the oxidation. The thickness of the oxidized film was estimated. Accordingly, the layer-by-layer oxidation was limited to approximately 50 nm via plasma irradiation, whereas the TaS2 films within 150 nm were fully oxidized via thermal annealing in ambient air. Therefore, a Ta-oxide/TaS2 structure was fabricated as a stack material of insulator and metal when the thickness of the pristine film was greater than 50 nm. In addition, Ta-oxide films were integrated into bottom-gated two-dimensional (2D) field-effect transistors (FETs) using the dry transfer method. 2D FETs with multilayer MoTe2 and MoS2 films as p-type and n-type channels, respectively, were successfully fabricated. In particular, the Ta-oxide film synthesized via dry oxidation was used as a gate dielectric, and the device process could be simplified because the Ta-oxide/TaS2 heterostructure can function as a stack material for gate insulators and gate electrodes. An anti-ambipolar transistor consisting of an MoTe2/MoS2 heterojunction was also fabricated. For the transfer characteristics, a relatively sharp on-state bias range below 10 V and sufficiently high peak-to-valley ratio of 106 at VDS= 3 V were obtained using the high-κ gate dielectric of Ta-oxide despite the presence of the multilayer channels (~ 20 nm).