Nd3+/Zr4+-cosubstituted bismuth titanate (BNTZx, x = 0, 0.05, 0.1, 0.3, and 0.5) thin films have been fabricated by chemical solution deposition and their polarization hysteresis loops, leakage current, and capacitance butterfly loops investigated. Results show that, at Zr content of x = 0.1, both capacitance and remanent polarization can be greatly improved. The BNTZ0.1 film also exhibits fatigue-free, excellent leakage current characteristics (I ≈ 9.44 × 10−9 A) at applied voltage of 3 V. High-quality c-axis-oriented BNTZx = 0.1 films with improved electrical properties were fabricated; this finding supports the feasibility of engineering polarization rotation in ferroelectric bismuth titanate (as suggested theoretically by Roy et al. in Appl. Phys. Lett. 102:182901, 2013).