Highly c-axis oriented Mg x Zn 1Àx O x ¼ 0 $ 0:2 ð Þ thin films with pure hexagonal phase were prepared on Pt/ TiO 2 /SiO 2 /Si substrates by chemical solution deposition method, and their structure, photoluminescence, and lattice vibrational properties were studied. For the thin films with Mg contents ranging 0≤x≤0.20, the room-temperature near-band-edge emission exhibited blueshift up to about 0.35 eV, indicating that the band-gaps of thin films could be tailored by Mg incorporation, meanwhile, the green emission of the thin films enhanced with increasing Mg content. Raman spectra analysis indicated that the decreasing high frequency E 2 Raman modes showed compositiondependent asymmetrically broadening. The difference of electronegativity between Mg 2+ for Zn 2+ as well as the potential fluctuation were discussed. Furthermore, longtitudial optical modes exhibited one-mode behavior with observed~25.8 cm −1 blueshift. X-ray photoelectron spectroscopy measurements clearly confirmed the Mg incorporation.