The growth of Ca-doped barium titanate thin films using a pulsed laser ablation technique were analyzed. The x-ray diffraction and scanning electron microscope studies revealed a polycrystalline nature with significant orientation along the (111) direction. The presence of a sharper interface was exhibited by the secondary ion mass spectrometer analysis. The results show that the dielectric constant and dielectric phase transition temperature of the thin films decreased with an increase in the calcium content.