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In this manuscript, for the first time, the exploration of the microstructural, ferroelectric, piezoelectric, and dielectric performances are measured for Sm-ion-influenced pseudo-cubic, morphotropic phase boundary (MPB) regional 0.62BiFeO₃−0.38SrTiO₃:xwt%Sm₂O₃ (BFST:xSm) ceramics with x = 0–0.25. All the compositions maintained their pseudo-cubic MPB structural stability. The composition of BFST:0.15Sm ceramics exhibited an excellent remnant polarization (<i>P_r</i>) of ~52.11 μC/cm², an enhanced <i>d₃₃</i> of 101 pC/N, and the highest relative dielectric constant (<i>ɛ_r</i>) of ~1152, which are much improved as compared to that of pure BFST ceramics. BFST:0.15Sm ceramics demonstrated a Curie temperature (<i>T_C</i>) of 378 °C. Moreover, the composition exhibited high thermal stability for <i>d₃₃</i> 72 pC/N (only a 28% decrease), even at a high temperature of 300 °C. Such outstanding outcomes make BFST:0.15Sm ceramics an ideal applicant for high-temperature piezoelectric applications.