We have reported the Raman spectroscopic measurements on the pellets of (Bi1-xSbx)2Te3 (x = 0 to 0.9) topological insulators. Raman spectra show the strong peak intensity of Raman active modes, A1g1 (∼92 cm−1), Eg2 (∼121 cm−1) and A1g2 (∼141 cm−1), for all the Sb contents besides the A1u1 (∼100 cm−1), IR-active mode, for x = 0.2 and 0.3. These out-of-plane (A1g1 and A1g2) and in-plane (Eg2) bond vibrational modes corresponding to the Bi/Sb–Te1 bonds are observed in (Bi1-xSbx)2Te3. For the higher Sb contents (x = 0.6 and 0.9) the bond vibrational mode shifts from Bi/Sb–Te1 (A1g1 and A1g2) to Bi–Sb (A1g1) and Sb–Te (A1g2) bonds. The A1g1 mode shifts towards the lower frequencies lead to a redshift as compared to that in pure Bi2Te3. The Raman active, A1g1, Eg2 and A1g2, modes show the strong electron-phonon interactions, disorder-induced inhomogeneous broadening, and interlayer interactions within quintuple layers.