A novel high-k gate dielectric material, i.e., hafnium-doped tantalum oxide (Hf-doped TaOx), has been studied for the application of the future generation metal-oxidesemiconductor field effect transistor (MOSFET). The film's electrical, chemical, and structural properties were investigated experimentally. The incorporation of Hf into TaOx impacted the electrical properties. The doping process improved the effective dielectric constant, reduced the fixed charge density, and increased the dielectric strength. The leakage current density also decreased with the Hf doping concentration. MOS capacitors with sub-2.0 nm equivalent oxide thickness (EOT) have been achieved with the lightly Hf-doped TaOx. The low leakage currents and high dielectric constants of the doped films were explained by their compositions and bond structures. The Hf-doped TaOx film is a potential high-k gate dielectric for future MOS transistors. A 5 A?A? tantalum nitride (TaNx) interface layer has been inserted between the Hf-doped TaOx films and the Si substrate to engineer the high-k/Si interface layer formation and properties. The electrical characterization result shows that the insertion of a 5 A?A? TaNx between the doped TaOx films and the Si substrate decreased the film's leakage current density and improved the effective dielectric constant (keffective) value. The improvement of these dielectric properties can be attributed to the formation of the TaOxNy interfacial layer after high temperature O2 annealing. The main drawback of the TaNx interface layer is the high interface density of states and hysteresis, which needs to be decreased. Advanced metal nitride gate electrodes, e.g., tantalum nitride, molybdenum nitride, and tungsten nitride, were investigated as the gate electrodes for atomic layer deposition (ALD) HfO2 high-k dielectric material. Their physical and electrical properties were affected by the post metallization annealing (PMA) treatment conditions. Work functions of these three gate electrodes are suitable for NMOS applications after 800A?A?C PMA. Metal nitrides can be used as the gate electrode materials for the HfO2 high-k film. The novel high-k gate stack structures studied in this study are promising candidates to replace the traditional poly-Si-SiO2 gate stack structure for the future CMOS technology node.