Orientation-engineered (La, Ce) cosubstituted 0.94(Bi0.5Na0.5)TiO3-0.06BaTiO(3) thin films were epitaxially deposited on CaRuO3 buffered (LaAlO3)(0.3)(Sr2AlTaO6)(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=29.5C/cm(2) and coercive field E-c=7.4kV/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.