Bilayer Ba0.6Sr0.4TiO3 - Ba0.4Sr0.6TiO3 and Ba0.4Sr0.6TiO3 - Ba0.6Sr0.4TiO3 thin films were deposited on the LaNiO3-buffered Pt/Ti/SiO2/Si substrates using pulse laser deposition method. A (100)preferred orientation was obtained. The structure was characterized using x-ray diffraction (XRD) and Raman spectroscopy. The leakage current, and dielectric permittivity versus temperature were characterized. Results indicated that the (100) preferred bilayer structure had less leakage current and smaller loss tangent, which was in favor of enhancing the quality of thin film used as microwave dielectrics.