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The development of piezoelectric ceramics characterized by both large piezoelectric response and high-temperature stability is imperative for the advancement of practical electromechanical devices. However, existing high-performance piezoelectric ceramics often encounter compromised temperature stability because ferroelectric phase transitions occur within low-temperature regions. In this work, we focused on Sm-doped Pb(Ni1/3Nb2/3)O3–PbZrO3–PbTiO3 (PNN–PZT:Sm) ceramics with a tetragonal (T)-phase structure to achieve the desired combination of high piezoelectricity and high temperature stability. The results indicate that 2 mol% Sm-doped samples exhibit a large piezoelectric constant (d33) of 575 pC/N, an effective piezoelectric strain coefficient (d33*) of 890 pm/V, and a high ferroelectric-to-paraelectric phase transition temperature (Tm) of 279 °C. Remarkably, d33 experiences only a 2.6% variation over the temperature range of 30–250 °C, while d33* changes by 8% within the temperature range of 30–180 °C. Microstructural and domain structure analyses suggest that Sm-doping effectively reduces the grain size, leading to a decreased domain size, thereby achieving excellent electromechanical properties. The superior temperature stability is attributed to the suppressive effect of Sm-doping on the R–T ferroelectric phase transition. These studies suggest that Sm-doping represents an effective strategy for achieving the collaborative optimization of piezoelectricity and temperature stability through grain and domain engineering techniques for perovskite ferroelectric materials.
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