We report a new approach to integrating high-k{appa} dielectrics in both bottom- and top-gated MoS2 field-effect transistors (FETs) through thermal oxidation and mechanical assembly of layered twodimensional (2D) TaS2. Combined X-ray photoelectron spectroscopy (XPS), optical microscopy, atomic force microscopy (AFM), and capacitance-voltage (C-V) measurements confirm that multilayer TaS2 flakes can be uniformly transformed to Ta2O5 with a high dielectric constant of ~ 15.5 via thermal oxidation, while preserving the geometry and ultra-smooth surfaces of 2D TMDs. Top-gated MoS2 FETs fabricated using the thermally oxidized Ta2O5 as gate dielectric demonstrate a high current on/off ratio approaching 106, a subthreshold swing (SS) down to 61 mV/dec, and a field-effect mobility exceeding 60 cm2V-1 s-1 at room temperature, indicating high dielectric quality and low interface trap density.