A high‐k, zirconium‐aluminum‐oxide (ZAO) gate insulator (GI) using low‐cost spray pyrolysis technique for large area and low power electronics is demonstrated. The high‐quality spray‐pyrolyzed ZAO GI is obtained with subsequent oxidation by eco‐friendly Ar/O2 plasma treatment. Analyses reveal that only one cycle Ar/O2 plasma treatment significantly enhances the thin‐film and dielectric properties of ZAO, exhibiting improved mass density (4.16 g cm−3), smooth surface roughness (0.32 nm), low leakage current density (2.26 × 10−6 A cm−2), high breakdown electric field (5.15 MV cm−1), and negligible frequency‐dependent capacitance. Hysteresis free, amorphous indium‐gallium‐zinc‐oxide (a‐IGZO) thin‐film transistors (TFTs) with ZAO GI exhibit a field‐effect mobility of 15.04 cm2 V−1 s−1, threshold voltage of 1.46 V, subthreshold swing of 115 mV dec−1, ION/IOFF ratio of 7.54 × 108, and negligible positive bias stress. The highly reliable a‐IGZO TFTs performances are achieved due to the significant reduction of oxygen‐related defects at the dielectric/semiconductor interface. The TFT inverter and an eleven‐stage ring oscillator have been demonstrated with ZAO/a‐IGZO TFTs, exhibiting a high voltage gain of 58, oscillation frequency of 2.43 MHz, and signal propagation delay of 18.7 ns at a supply voltage of 6 V, confirming the benefit of spray‐pyrolyzed high‐k ZAO dielectric for low power displays.