Ferroelectric thin films of bismuth-containing layered perovskite SrxPbyBi2zTa2O9 have been prepared using the metalorganic decomposition method. The effect of both Sr and Pb content on the crystal structure, microstructure, and ferroelectric properties of SrxPbyBi2.3Ta2O9 films was investigated. A maximum remanent polarization of 2Pr=19.2μC/cm2 was obtained for the SrxPb0.2Bi2.3Ta2O9 film with 20 mol % Sr-deficient composition as prepared at 800°C, which could be the compromising effects of Sr content on both grain growth and second phase formation of BiTaO4. The substitution of Pb for Bi is accompanied by the occurrence of oxygen vacancies to compensate the charge balance, which is responsible for grain growth mechanism in Sr0.8Pb0.2Bi2.3Ta2O9 films. Fatigue endurance of Sr0.8Bi2.3Ta2O9 films becomes problematic after 109 cycles with a decrease in remanent polarization to 85% of the original value. This phenomenon was related to electron injection and creation of electron traps due to the occupation of Sr vacancies by Bi cations. It is demonstrated that the fatigue endurance of Sr0.8Bi2.3Ta2O9 film can be improved by doping with 20 mol % PbO.