This study describes the microstructure, crystal structure, dielectric and piezoelectric behavior of 0.1Pb[Fe 1/2 Nb 1/2 ]O 3 -0.9Pb[Zr x Ti (1-x) ]O 3 (x = 0.49-0.55) ceramics synthesized by solid-state reaction. Compositions were sintered at 1180 o C for 120 min. Dense and uniform microstructure was seen through microstructural analysis. XRD pattern confirmed the co-existence of tetragonal and rhombohedral perovskite phases in these compositions where 0.51 x 0.53. Compositions with 0.51 x 0.53 resulted in the optimum values of properties, viz. dielectric constant ( r ) of 1150, piezoelectric coefficient (d 31 ) of 9510 -12 C/N, piezoelectric voltage constant (g 31 ) of 7010 -3 mV/N and the coupling factor (k p ) value of 0.67. Results indicated that this material composition could be suitable for power harvesting and sensor applications.