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Solution deposition of high-quality dielectric films is one of the big challenges in achieving excellent electrical performance of bi-layer solution-processed metal oxide (MO) thin film transistors (TFTs). Using an oxygen-doped precursor solution (ODS), we successfully deposited high-quality zirconium oxide (ZrO2) dielectric films by a solution process. The ODS-ZrO2 films show low leakage current density (10−7 A cm−2 at 2 MV cm−1), high breakdown electric field (7.0 MV cm−1) and high permittivity (19.5). Consequently, solution-processed indium oxide (In2O3) TFTs with ODS-ZrO2 film as the gate dielectric show excellent electrical performance, for example high carrier mobility up to 62.02 cm2 V s−1, a large on/off drain current ratio of 3.0 × 106, a small subthreshold swing of 0.14 V and excellent bias stress stability. Our work demonstrates the critical role of the dielectric film in the electrical performance of MO-TFTs. More importantly, we reveal that high dielectric constant (κ) dielectric film deposited with ODS should be an effective way to significantly increase the electrical properties of MO-TFTs for future low-cost, high-performance applications. [ABSTRACT FROM AUTHOR]