Orientation-engineered (La, Ce) cosubstituted 0.94(Bi 0.5 Na 0.5 ) TiO 3 -0.06BaTiO 3 thin films were epitaxially deposited on CaRuO 3 buffered (LaAlO 3 ) 0.3 (Sr 2 AlTaO 6 ) 0.35 single-crystal substrates by pulsed laser deposition. The ferroelectric, piezoelectric, dielectric, and leakage current characteristics of the thin films were significantly affected by the crystallographic orientation. We found that the (001)-oriented film exhibited the best ferroelectric properties with remnant polarization P r = 29.5 lC/cm 2 and coercive field E c = 7.4 kV/mm, whereas the (111)-oriented film demonstrated the largest piezoelectric response and dielectric permittivity. The bipolar resistive switching behavior, which is predominantly attributed to a combined effect of ferroelectric switching and formation/rupture of conductive filaments, was observed. The conduction mechanisms were determined to be ohmic conduction and Poole-Frenkel emission at high-and low-resistance states, respectively, in all the films. †