The development of piezoelectric ceramics with both large piezoelectric responses and mechanical quality factor is still a key challenge for practical applications for high-power piezoelectric devices. Here we report the strategy to utilize the synergistic contribution of engineered defect and domain structure, in which an excellent piezoelectric coefficient d 33 of 655 pC N −1 and mechanical quality factor Q m of 371 are simultaneously achieved in MnCO 3 -modified Pb(Ni,Nb)O 3 -PbZrO 3 -PbTiO 3 (Mn-PNN-PZ-PT) ceramics. Meanwhile, the depolarization temperature (T d ) and the temperature corresponding to the ε r,max (T m ) are enhanced relative to the pure counterpart. After annealing at 90 • C, the sample with x = 0.3 shows the retained d 33 value of 610 pC N −1 , about 2.6 times larger than that with x = 0 counterpart, demonstrating a wider operating temperature range. These enhanced electromechanical properties originate from the internal bias field introduced by the defect dipoles (Mn ′′ Zr,Ti − 𝑉 •• O ) 𝑋 and (Mn ′′′ Nb − 𝑉 •• O ) ′ . It is verified that xMn-PNN-PZ-PT ceramics have superior potential for highpower application, meanwhile, paves a significant step toward enhancing the thermal stability of high-temperature piezoceramics.