As electronic circuit integration intensifies, there is a rising demand for dielectric insulators that provide both superior insulation and high dielectric constants. This study focuses on developing high-k dielectric insulators by controlling the phase of the Hf0.5Zr0.5O2 (HZO) film with additional doping, utilizing yttrium (Y), tantalum (Ta), gallium (Ga), silicon (Si), and aluminum (Al) as dopants. Doping changes the ratio of tetragonal to monoclinic phases in doped HZO films, and Y-doped HZO (Y:HZO) films specifically exhibit a high tetragonal phase ratio and a dielectric constant of 40.9, indicating superior insulating properties compared to undoped HZO films. To clarify the fundamental mechanism driving the enhancement in dielectric properties, we have carried out various analyses combined with density functional theory (DFT) calculations. Through the optimization of the post-deposition annealing (PDA) process and the heterojunction structure with Al2O3, an Al2O3/Y:HZO heterojunction with a high dielectric constant and even lower leakage current compared to a single layer was developed. The thin-film transistor (TFT) with the Au/Ti/amorphous InGaZnO4 (a-IGZO)/Al2O3/YHZO/TiN heterojunction structure exhibits low subthreshold swing (SS) values within a narrow gate-source voltage (Vsg) range. This study advances knowledge on how the controlled-phase doped HZO films affect the dielectric constant and leakage current and will contribute to semiconductor technology advancements by overcoming the limitations of conventional high-k dielectric insulators.