© 2018 Elsevier B.V.We experimentally and theoretically study how the structural and vibrational properties of zinc oxide (ZnO) are modified upon Gallium (Ga) doping. The characteristics of Ga-doped ZnO thin films which are synthesized by sol-gel spin coating method on glass substrates are monitored by using X-ray diffraction (XRD) and Raman scattering measurements. For atomic-level understanding of the experimental findings state-of-the-art density functional theory (DFT) based calculations are also performed. DFT calculations reveal that both the substitution and adsorption of Ga atoms in ZnO are energetically possible and substitutional doping in ZnO is the most favourable scenario. XRD measurements show that all the films are in wurtzite structure and the crystallite size of the films decreases with increasing Ga doping. In addition, Raman analysis show that strong vibrational modes at about 100 and 441 cm−1 are associated with E2 low and E2 high phonon branches of ZnO, respectively. While the frequency of the E2 low mode downshifts with increasing Ga concentration, the E2 high phonon mode is not affected by the Ga doping. Furthermore, EGa phonon branch, stemming from the substituted Ga atoms, emerges at low frequencies. It is also seen that the Raman intensity of the EGa peak linearly increases with increasing Ga concentration. Experimental results on the vibrational properties are in good agreement with the ab initio phonon calculations.