The relationships between the microstructure and the dielectric properties of sol–gel prepared Y2O3 films with various Gd3+ doping were systematically investigated. Robust solution processed lanthanide films, (Y1−xGdx)2O3
(0 < x ≤ 0.5), are demonstrated as high-k gate insulators for low voltage-driven oxide thin film transistors and their optimized composition is presented. With the proper amount of Gd3+ doping, the corresponding thin film insulators exhibit low leakage current with
increased dielectric constant. The resultant Zn–Sn–O/(Y, Gd)2O3 TFT exhibits enhanced performance, by a factor of 10.7 compared with TFTs using a SiO2 insulator, with a field-effect mobility of ~3.15 cm2V−1s−1 and
an exceptionally low operating voltage <15 V.