A high-performance piezoelectric material, 0.95Pb(Zr_0.52Ti_0.48)O₃-0.05Pb(Mn_1/3Nb_2/3)O₃ (PZT-PMnN) ceramic, was prepared by using a spark plasma sintering (SPS) method. By systematically comparing the electrical properties, the spark-plasma-sintered sample was demonstrated to be superior to a conventionally sintered sample. With respect to conventionally sintered ceramic, the d₃₃ of spark-plasma-sintered ceramic increases from 323 pC/N to 412 pC/N, and the increases from 318 pm V⁻¹ to 553 pm V⁻¹. More importantly, the mechanical quality factor (Q_m) reaches 583, which is three times higher than the conventionally sintered sample (Q_m ∼ 182). Furthermore, the SPS method was found to be capable of promoting other electrical properties simultaneously. Therefore, the SPS method is proposed to be an effective processing method to fabricate PZT-PMnN ceramics of higher performance.