Using a new composite flux and an improved growth process, large and high-quality ferroelectric SrBi2Ta2O9 (SBT) single crystals (up to 25 × 20 mm2 area) were successfully grown from high-temperature solutions. The effects of chemical, thermodynamic, and kinetic parameters on the growth results were systematically studied. The optimum system for the growth of SBT crystals has been identified. B2O3 additive was shown to play an important role in improving the effectiveness of the Bi2O3 solvent. The grown SBT single crystals exhibit a dominant (001)-orientation and large single-domain areas. The dielectric and ferroelectric properties measured in relation to crystal orientations have confirmed the absence of any polarization component normal to the (Bi2O2)2+ sheets of the structure, indicating a high anisotropy in the properties.