Recently, piezoelectric devices, such as ultrasonic surgery, ultrasonic atomizer, and ultrasonic speaker, are analyzed and designed by finite element simulation methods. However, the discrepancy between the design and the experiment results of the device typically occurs due to the inaccuracy of the piezoelectric material properties. To improve the simulation accuracy, the material properties of the PZT ceramics were better refined using parameter estimation method. The material parameters are elastic stiffness c^E_ij and piezoelectric constant e_ij of PZT ceramics. The impedance curve characteristics for the LTE mode of PZT ceramics were calculated. The mismatch between the simulation and the experimental data were compared and minimized by a least square method. Finally, the simulated impedance data were compared with the experimental data for the various vibration modes of PZT ceramics and the optimized material properties of PZT ceramics were verified. To further verify the accuracy, this method was also applied to piezoelectric PMN-PT single crystals.