In this study, (Cr 1/3 /Ta 2/3 ) non-equivalent co-doped Bi 4 Ti 3 O 12 (BIT) ceramics were prepared to solve the problem that high piezoelectric performance, high Curie temperature, and high-temperature resistivity could not be achieved simultaneously in BIT-based ceramics. A series of Bi 4 Ti 3−x (Cr 1/3 Ta 2/3 ) x O 12 (x = 0-0.04) ceramics were synthesized by the solid-state reaction method. The phase structure, microstructure, piezoelectric performance, and conductive mechanism of the samples were systematically investigated. The B-site non-equivalent co-doping strategy combining high-valence Ta 5+ and low-valence Cr 3+ significantly enhances electrical properties due to a decrease in oxygen vacancy concentration. Bi 4 Ti 2.97 (Cr 1/3 Ta 2/3 ) 0.03 O 12 ceramics exhibit a high piezoelectric coefficient (d 33 = 26 pC•N −1 ) and a high Curie temperature (T C = 687 ℃). Moreover, the significantly increased resistivity (ρ = 2.8×10 6 Ω•cm at 500 ℃) and good piezoelectric stability up to 600 ℃ are also obtained for this composition. All the results demonstrate that Cr/Ta co-doped BIT-based ceramics have great potential to be applied in high-temperature piezoelectric applications.