The control of the correlated state in complex oxides offers the opportunity to harness the multifunctional properties characteristic of these systems, one example of which is the recent observation of multiferroic behavior in Pb(Zr0.2Ti0.8)O-3/La1-xSrxMnO3 (PZT/LSMO) heterostructures. Here, the authors present a detailed study of the growth and structural characterization of epitaxial PZT/LSMO structures grown by a combination of molecular beam epitaxy and off-axis rf magnetron sputtering. In situ and ex situ structural characterizations demonstrate the high quality and single crystalline nature of the films over a wide range of film compositions and thicknesses. (C) 2010 American Vacuum Society. [DOI: 10.1116/1.3427140]