SrBi2Ta2O9 (SBT) thin films were deposited onto Pt/Ti/SiO2/Si substrates by liquid-delivery metal–organic (MO) CVD using Sr[Ta(OC2H5)5(OC2H4OCH3)]2 and Bi(C6H5)3 precursors. The film composition was primarily controlled by varying the deposition temperature and the concentration of the single-mixture solution. The stoichiometric SBT thin films deposited at 540 °C were well crystallized, and showed a relatively high intensity of α-axis orientation of (200), as well as the main peaks of (115) and (008). The SBT films, annealed at 750 °C in ambient oxygen showed a good ferroelectric property, a saturated hysteresis loop even at an applied voltage of 2 V. The remanent polarization (2 Pr) and coercive field (Ec) of SBT films annealed at 750 °C were 12 μC cm−2 and 60 kV cm−1, respectively, at an applied voltage of 5 V.