Ferroelectric lead bismuth titanate (PbBi4Ti4O15) thin films, selectively controlled in c-axis and off-c-axis orientation, were fabricated on a Pt layer by a chemical solution deposition method. The off-c-axis oriented PbBi4Ti4O15 films demonstrated much higher remanent polarization (8.7 μC/cm2) than those of c-axis oriented films (3.7 μC/cm2). Regardless of grain orientation, PbBi4Ti4O15 films were not fatigued up to 1010 cycles under 9-V application. It is deduced that the role of Bi2O22+ layer in inducing fatigue-free property for this Bi-layered perovskite structure is the self-regulation of space charge.