Abstract We have successfully grown in situ, by laser ablation, the following heterostructures: Pb(Zr0.52Ti0.48)O3 / YBa2Cu3O7 / CeO2 / (1102) Al2O3(PZT/YBCO/CeO2/Al2O3), Pb(Zr0.52Ti0.48)O3 / YBa2Cu3O7 / (100) SrTiO3(PZT/YBCO/STO), and Pb(Zr0.52Ti0.48)O3 / SrTiO3 / (100) MgO (PZT/STO/MgO). By combining RHEED. x-ray diffraction and atomic force microscopy, we have determined that (a) all the buffer and electrode layers are atomically flat, (b) PZT grows in the 2D to 3D Stransky-Krastanov mode, (c) there is an epitaxial relationship between the in-plane axes of the layers and the substrates, and (d) the c-axis of PZT is perpendicular to the plane of the film. Raman scattering shows a significant difference in spectra between a PZT thin film heterostructure and a ceramic PZT target. This is further evidence for the epitaxial nature of the PZT films and their fundamental difference with respect to ceramic samples.