Ferroelectric ceramics derived from the solid solution of (1-x)PbTiO₃-xBiAlO₃ (x = 0, 0.05, 0.10, 0.15, and 0.18) have been synthesized by solid-state reactions. A pure perovskite phase is formed for 0 ≤ x ≤ 0.15. The tetragonality (c/a) of the solid solution decreases with the increasing amount of BiAlO₃. Scanning electron microscopic images reveal a microstructure with a fine grain size of less than 1 μm for the solid solution ceramics (x ≥ 0.05). Compared with pure PbTiOPbTiO₃ ceramics whose high conductivity and poor densification were harmful to their dielectric performance, the ceramics of (1-x)PbTiO₃-xBiAlO₃ are well-densified (with a relative density of up to 93%) and their dielectric and ferroelectric properties are significantly improved with the addition of BiAlO₃, exhibiting reduced dielectric losses, well-developed P-E hysteresis loops (for x = 0.05, 0.10, and 0.15) and a high remnant polarization (P(r)) of 64 μC/cm² (for x = 0.15).