This paper aims at the determination of the effects of strontium addition on the microstructural evolution and the piezoelectric properties for Pb(Mn1/3Nb2/3)O3-Pb(Zr,Ti)O3 (PMnN-PZT) ceramics. The Sr content was chosen in the range of 2-8 mol%. These materials were prepared by the solid phase reaction of the oxides. It was found, from the experimental results, the tetragonality of the PMnN-PZT lattice and the Curie temperature decreased with Sr content; in the meantime, dielectric constant increased greatly. Dielectric constant (er) and planar coupling factor (Kp) was proven to be dependent on sintering temperature. P-E curves of PMnN-PZT system exhibited some “pinched” shape instead of the normal square-like P-E loops, illustrating presence of the oxygen vacancies by reason of the preferable substitution of the B-sites ion.