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Cobalt-modified 0.40Bi(Sc_3/4In_1/4)O₃–0.58PbTiO₃–0.02Pb(Mg_1/3Nb_2/3)O₃ ceramics (abbreviated as BSI–PT–PMN–<i>x</i>Co) were produced by conventional two-step solid-state processing. The phase structure, micro structure morphology, and electrical properties of BSI–PT–PMN–<i>x</i>Co were systematically studied. The introduction of Co ions exerted a significant influence on the structure and electrical properties. The experiment results demonstrated that Co ions entered the <i>B</i>-sites of the lattice, resulting in slight lattice distortion and a smaller lattice constant. The average grain size increased from ~1.94 μm to ~2.68 μm with the increasing Co content. The optimized comprehensive electrical properties were obtained with proper Co-modified content 0.2 wt.%. The Curie temperature (<i>T</i>_c) was 412 °C, the piezoelectric constant (<i>d</i>₃₃) was 370 pC/N, the remnant polarization (<i>P</i>_r) was 29.2 μC/cm², the relatively dielectric constant (<i>ε</i>_r) was 1450, the planar electromechanical coupling coefficient (<i>k</i>_p) was 46.5, and the dielectric loss (tan<i>δ</i>) was 0.051. Together with the enhanced DC resistivity of 10⁹ Ω cm under 300 °C and good thermal stability, BSI–PT–PMN–0.2Co ceramic is a promising candidate material for high-temperature piezoelectric applications.