Lanthanide (Ln) doping of lead zirconate titanate (PLnZT 4/30/70) thin films was conducted to investigate effects on structural and electrical properties. Films were spin-coat deposited from precursor solutions made using a previously reported “basic route to PZT” chemistry. The remanent polarization (Pr), dielectric constant (ε), dielectric loss (tan δ), and lattice parameter values were obtained for each of the doped PLnZT films. Films doped with amphoteric cations (Tb, Dy, Y, and Ho) displayed high Pr values, square hysteresis loops, and enhanced fatigue resistance. Smaller radius Ln-doped films display an increased tendency toward (100) orientation in otherwise (111)-oriented films.