We report the application of ambient spray pyrolysis for the deposition of high-k polycrystalline Y2O3 and amorphous Al2O3 dielectrics and their use in low-voltage ZnO thin-film transistors. The films are studied by means of atomic force microscopy, UV-visible absorption spectroscopy, impedance spectroscopy, and field-effect measurements. ZnO transistors based on spray pyrolysed Y2O3 and Al2O3 dielectrics show low leakage currents, and hysteresis-free operation with a maximum electron mobility of 34 cm(2)/V s and current on/off ratio on the order of 10(5). This work is a significant step toward high-performance oxide electronics manufactured using simple and scalable processing methods.