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Multilayered doped BaTiO3 thin films have been fabricated by physical vapor deposition (PVD) on low-cost polycrystalline substrates with the aim to improve dielectric properties by controlling point charge defects at the interfaces. We show that carefully designed interfaces lead to increasing the relative permittivity of the BaTiO3 thin films, in contradiction with the common belief that interfaces behave as dead layers. High relative permittivity up to 1030 and tanδ = 4% at 100 kHz and room temperature were obtained on BaTiO3 multilayered films deposited on Si/Pt substrates by PVD. The large permittivity is suspected to be an extrinsic contribution due to band bending at the interfaces, as inferred by in-situ X-ray photoelectron spectroscopy. A 20-nm depletion layer was found to be associated with an interdiffusion of dopants, as measured by depth profiling with time-of-flight secondary ion mass spectrometry. The films exhibit high permittivity and low dielectric losses stable between 200 and 400 K, which meet the requirement of electronic applications.