Studies performed by our group on composition-structure-property relationships of Pb(ZrxTi1−x)O3(PZT)-based heterostructure capacitors are reviewed. The work discussed is related to the synthesis and characterization of ferroelectric PZT and conductive Pt, RuO2, and La0.5Sr0.5CoO3layers and their integration into heterostructure capacitors suitable for non-volatile memories. The main objective of our research was to determine the influence of deposition parameters and layer processing on the composition, structure, and properties of PZT-based capacitors, with the goal of controlling fatigue, retention, and imprint effects. The work discussed relates mainly to the synthesis of films by ion beam sputter-deposition (IBSD) and pulsed laser ablation deposition (PLAD), where the heterostructures are grownin-situwithout exposing the interfaces to uncontrollable atmospheric conditions. Limited comparisons are presented between structural characteristics and properties of PZT capacitors produced by IBSD and PLAD and those synthesized by the sol-gel technique.