This investigation presents the growth of (100), (110) and preferential (111)-oriented Pb0.6Sr0.4TiO3 thin films prepared on different orientations LaNiO3 buffered silicon substrates via radio-frequency magnetron sputtering method. The effects of the orientation on microstructure and dielectric response were systematically investigated. The capacitance-voltage property versus the crystallographic orientation analysis revealed that preferential (111)-orientation film possesses the largest relative permittivity and tunability of 1180 and 84% (at 400 kV/cm) respectively, which are much higher than those of (100)- and (110)-oriented thin films. These results suggest preferential (111)-orientation films as promising candidates for microwave tunable devices. (C) 2013 Elsevier B.V. All rights reserved.