Pb(Zr, Ti)O3 (PZT) thin films were deposited on Pt/SiO2/Si substrates by metalorganic chemical vapor deposition using solid delivery system. The effects of deposition parameters such as the substrate temperature, the concentration of Pb precursor in the precursor mixtures, and the reactor pressure on the structural and electrical properties of PZT thin films were investigated. To obtain single-phase PZT thin films, the optimal range of the substrate temperature should be between 600 and 650 °C. The PbO content in PZT thin films was proportional to the fraction of Pb in the precursor mixture below 550 °C, but it was independent of the fraction of Pb in the mixture above 600 °C. With the increment of the reactor pressure, Zr contents in PZT thin films were increased, and the Pb/(Zr + Ti) ratio became more stoichiometric so that the ferroelectric properties were improved.