Elemental depth profiles of PZT films prepared by two sol–gel formulations, differing in the zirconium precursor stabilization, were investigated by SIMS analysis. Early decomposition of the zirconium precursor yielded opposing gradients of zirconium and titanium, while simultaneous late decomposition of zirconium and titanium precursors provided profile uniformity. The gradients formed during initial crystallization are irreversible. Both types of films showed excellent hysteresis; however, uniform films exhibited a much higher dielectric constant, indicating superior piezoelectric properties. Non-uniform films displayed a complex CV pattern, consistent with an inhomogeneous structure. Finally, thermal decomposition of the individual metal precursors is crucial for controlling film uniformity.