Mn/Y co-doped Ba 0.67 Sr 0.33 TiO 3 (BST: Mn+Y) thin films were deposited on LaNiO 3 (LNO)/SiO 2 /Si substrates by radio frequency (RF) magnetron sputtering technique, and the films were annealed subsequently at different temperatures. X-ray diffraction (XRD) demonstrated that all films are polycrystalline with a perovskite structure. Scanning electron microscopy (SEM) investigations revealed that all the films have dense and crack-free surface. The BST: Mn+Y films annealed at 700 • C showed the best electrical properties, with a dielectric constant of 855, dielectric loss of 0.032, tunability of 60% at room temperature and 100 kHz, and the remnant polarization of 7.1 μC/cm 2 and the leakage current density of 1.3 × 10 −4 A/cm 2 at an electric field of 400 kV/cm, respectively. The results reveal that microstructure plays an important role in enhanced electrical properties of the BST: Mn+Y thin films.