Due to its endurance to ferroelectric fatigue, SrBi2Ta2O9 (SBT) has been extensively investigated. We report here the synthesis of Sr1−xBaxBi2Ta2O9 (x = 0.0, 0.1, 0.5, 1.0) using a solution-based route. The precursors used in this work were the salts of strontium, barium, bismuth, and tantalum ethoxide. X-ray diffraction and Raman spectroscopic studies indicated the formation of complete solid solution system for Sr1−xBaxBi2Ta2O9. This material system may provide interesting properties relevant to microwave tuning and ferroelectric memory applications, which are under investigation.