In this study, the electrical properties of Bi4Ti3O12‐based Aurivillius‐type ceramics were tailored by a B‐site co‐doping strategy combining high valence Ta5+ and low valence Cu2+. A series of Bi4Ti3−x(Cu1/3Ta2/3)xO12 (BTCT) (x = 0, 0.005, 0.01, 0.015, 0.02, 0.025, and 0.03) ceramics were prepared by the conventional solid‐state reaction method. The effect of Cu/Ta co‐doping on the crystal structure, microstructure, dielectric properties, piezoelectric properties, ferroelectric properties, and electrical conductivity of these ceramics was systematically investigated. Co‐doping significantly enhanced the piezoelectric properties and DC electrical resistivity of the resulting composites. The optimized comprehensive performances were obtained at x = 0.015 with a large piezoelectric coefficient (34 pC/N) and a relatively high resistivity of 9.02 × 106 Ω cm at 500°C. Furthermore, the ceramic also exhibited stable thermal annealing behaviors and excellent fatigue resistance. The results of this study demonstrated great potential of the Cu/Ta co‐doped Bi4Ti3O12 ceramics for high‐temperature piezoelectric device applications.