Abstract: This study described the structural, dielectric, and piezoelectric behavior of Pb_1−xSr_x (Zr_0.52Ti_0.48)_0.95(Mn_1/3Nb_2/3)_0.05O₃ ceramics (PSZT-PMN, x = 0, 0.025, 0.050, and 0.075), prepared by a semi-wet route. X-ray diffraction, dielectric, and piezoelectric investigations were carried out to analyze the crystal structure. The relative dielectric constant and dielectric loss were both calculated as the functions of temperature. The room-temperature dielectric constant reaches a maximum for a Sr²⁺-modified PZT-PMN ceramic with an x value of 0.050, which corresponds to the morphotropic phase boundary (MPB). Raman spectroscopy studies also confirm the existence of this MPB for x = 0.050. The piezoelectric strain coefficients (d₃₃) value shows a maximum response for this composition. In addition, the phase transition temperature decreases significantly when the Sr²⁺ concentration increases in the PZT-PMN ceramics.