(1−x) Pb[Yb 1/2 Nb 1/2 ] O 3 –x PbTiO 3 (PYbN–PT, x=0.5) (001)-oriented thin films were deposited onto (111)Pt/Ti/SiO2/Si substrates by sol–gel processing. The crystallographic texture of the films was affected by heating rate, annealing temperature, and film thickness. The dielectric permittivity and loss factor varied only slightly with frequency in the range of 100 Hz–100 kHz. At 1 kHz, the dielectric permittivity of (001)-oriented films was 1030 and the dielectric loss was 0.03. Compared with (111)-oriented PYbN–PT films, (001)-oriented PYbN–PT films exhibited better piezoelectric properties. The effective transverse piezoelectric e31,f coefficient of the films were −8.2 C/m2 when films were poled at room temperature. Enhanced piezoelectric properties were observed by poling the films at higher temperatures. The transition temperature of the (001)-oriented PYbN–PT (50/50) films was around 360 °C.