Addition of calcium ion in La and Sr co-doped lead zirconate titanate (PLSZT) was investigated to improve the dielectric and piezoelectric properties of PLSZT system. Ca doped PLSZT was prepared using high energy planetary ball mill, pelletized and sintered at 1200 °C for 3 hours. XRD results showed that all Ca-doped PLSZT samples present perovskite structure with tetragonal phase. FESEM results showed that the grain size of the samples was decreased with increasing calcium composition but began to enlarge at 0.008 mol% of calcium. The density was observed to be slightly decreased as addition of calcium ion. The dielectric permittivity (Er) and piezoelectric coefficient (d33) and electromechanical coupling factor (kp) were increased with the composition of calcium up to 0.005 mol%.