Using the MOCVD process to produce Pb(Zr, Ti)O3 (PZT) thin films, control of the film stoichiometry and crystalline phase was achieved. The PZT films obtained showed good step coverage, 67%. Uniform PZT and PLZT thin films with a variation of film thickness of less than ±1.5% were successfully obtained on a 6–8 inch silicon wafer. For the evaluation of the crystallinity and epitaxial relationship of the PZT thin films, the total reflection X-ray diffraction (TRXD) method was used for the first time. Using TRXD, the in-plane orientations of PZT and Pt in PZT/Pt/MgO were evaluated. The growth mechanism of PbTiO3 and PZT thin films at the initial growth stage was also investigated using an atomic force microscope (AFM). The switching characteristics of PZT capacitors using Ir and IrO2 electrodes for memory device applications were also investigated and a PZT capacitor with no fatigue up to a switching cycle of 1011 was obtained.