With growing concern over world environmental problems and increasing legislative restriction on using lead and lead-containing materials, a feasible replacement for lead-based piezoceramics is desperately needed. Herein, we report a large piezoelectric strain (d33*) of 470 pm/V and a high Curie temperature (Tc) of 243 °C in (Na0.5K0.5)NbO3-(Bi0.5Li0.5)TiO3-BaZrO3 lead-free ceramics by doping MnO2. Moreover, excellent temperature stability is also observed from room temperature to 170 °C (430 pm/V at 100 °C and 370 pm/V at 170 °C). Thermally stimulated depolarization currents (TSDC) analysis reveals the reduced defects and improved ferroelectricity in MnO2-doped piezoceramics from a macroscopic view. Local poling experiments and local switching spectroscopy piezoresponse force microscopy (SS-PFM) demonstrates the enhanced ferroelectricity and domain mobility from a microscopic view. Distinct grain growth and improvement in phase angle may also account for the enhancement of piezoelectric properties.