We developed a simple and environmentally friendly spin-coating method for high-κ dielectrics (AlOx, ZrOx, YOx and TiOx). These materials were used as gate dielectrics for solution-processed nanocrystalline In2O3 or amorphous InZnO TFTs with a maximum processing temperature of 300 °C. The role of high-κ dielectrics in device performance was systematically studied. Among the high-κ dielectrics, the AlOx-based devices showed the best performance with mobilities of 21.7 cm2 V−1 s−1 in an In2O3 TFT and 11.6 cm2 V−1 s−1 in an InZnO TFT with the on/off current ratio exceeding 106. Furthermore, the devices exhibited ultra-low operating voltages (<3 V) and negligible hysteresis. A comprehensive study suggests that the high performance of the AlOx-based devices could be attributed to the smooth dielectric/semiconductor interface and the low interface trap density besides its good insulating properties. Therefore, the solution-processed AlOx can be used as a promising high-κ dielectric for low cost, low voltage, high-performance oxide electronic devices.