An organic–inorganic hybrid film is deposited from O2/HMDSO plasma. The SiOSi/SiCH3 FTIR absorption ratio of this film increases with the process power and O2/HMDSO precursor flow ratio, resulting in a more inorganic‐like film. This hybrid film is used as the gate dielectric of MgZnO TFTs. As the SiOSi/SiCH3 FTIR absorption ratio of the gate dielectric increases, the gate leakage current decreases, on/off current ratio increases, threshold voltage increases, and subthreshold swing increases. High SiCH3 bonding content in the gate dielectric improves TFT switching but deteriorates gate insulation, resulting in increased gate leakage current and decreased on/off current ratio.