For high-power on-resonant piezoelectric applications, piezoelectric materials with high piezoelectric coefficient (d33) and mechanical quality factor (Qm) are in high demand. However, previous work has shown that the d33 and Qm are generally inversely proportional, implying that it is difficult to improve these properties simultaneously. Here we report the simultaneous enhancement of d33 and Qm in (Mn, Zr) co-doped BaTiO3 (BT-xMn-yZr) ceramics. Compared with pure BaTiO3 ceramics, the piezoelectric coefficient (d33) of BT-0.5%Mn-5%Zr ceramic is increased from 190 pC/N to 321 pC/N, and the Qm is increased from 290 to 513. Furthermore, the Qm of BT-1%Mn-5%Zr ceramic reaches 1470, and the d33 is 248 pC/N. When both d33 and Qm are considered, the obtained properties outperform commercial hard Pb(Zr,Ti)O3 and other typical lead-free ferroelectric ceramics. The experimental results show that the enhanced d33 and Qm of these ceramics originate from the synergistic effect of defect engineering-induced domain configuration effect and pinning effect. This work provides insights into the design of high-performance high-power lead-free ferroelectric materials.