The interface layer between thin sputter-deposited tantalum oxide (TaOx) high-k film and silicon substrate was engineered with the Hf doping method and the insertion of a thin 5Å TaNx interface. The following results have been obtained: 1) the Hf dopant in the TaOx film was involved in the interface formation process, e.g., forming a new, thinner high-k HfSixOy interface layer rather than the SiOx layer, 2) when the TaNx interface was inserted, the interface layer composition was even more complicated, e.g., including TaOxNy and HfSixOy structures. No hafnium nitride or oxynitride was detected, 3) the interface layer structure was changed, e.g., from single-zone to multi-zone with different compositions, 4) when a low concentration of Hf existed in the TaOx film, the high-k dielectric properties, such as the k value, fixed charge density, dielectric strength, were improved, and 5) when the thin TaNx interface layer was inserted, the above electric properties were further improved. However, the fixed charge density and interface states were increased due to the insertion of the TaNx interface layer. These results were contributed by factors such as the charge-trapping characteristics in the interface layer and the some damage repairing mechanisms. In summary, this research proved that the high-k film's interface layer and bulk properties could be were improved with the doping process as well as the insertion of an ultra-thin TaNx interface film.