Thin films of ferroelectric (SrBi2Ta2O9)x(Bi3TiNbO9)1−x layered structure were prepared for x = 0.0, 0.2, 0.4, 0.6, 0.8, and 1.0, by metal organic solution deposition method on Pt/TiO2/SiO2/Si substrates. The micro-Raman studies reveal that the samples are mostly homogeneous. The Raman sprectrum for the film with x = 0 shows bands around 60, 170, 232, 256, 337, 569, and 839 cm−1, which indicate Bi3TiNbO9 (BTN) formation. The prominent band around 839 cm−1, which is an A1g mode of the orthorombic symmetry, corresponds to symmetric stretching of the BO6 octahedra. The frequency of this band is found to shift significantly as SrBi2Ta2O9(SBT) material is added to the BTN compound. In this paper, the evolution of the Raman bands with the inclusion of SBT material are presented and discussed. Finally, The Raman spectra of SBT- BTN films are compared with those obtained in SBT-BTN bulk ceramics.