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The quality of the gate dielectric/semiconductor interface in thin-film transistors (TFTs) is known to determine the optimum operating characteristics attainable. As a result in recent years the development of methodologies that aim to improve the channel interface quality has become a priority. Herein, we study the impact of the surface morphology of three solution-processed high-k metal oxide dielectrics, namely AlOx, HfOx, and ZrOx, on the operating characteristics of In2O3 TFTs. Six different dielectric configurations were produced via single or double-step spin-casting of the various precursor formulations. All layers exhibited high areal capacitance in the range of 200 to 575 nF/cm2, hence proving suitable, for application in low-voltage n-channel In2O3 TFTs. Study of the surface topography of the various layers indicates that double spin-cast dielectrics exhibit consistently smoother layer surfaces and yield TFTs with improved operating characteristics manifested, primarily, as an increase in the electron mobility (µ). To this end, µ is found to increase from 1 to 2 cm2/Vs for AlOx, 1.8 to 6.4 cm2/Vs for HfOx, and 2.8 to 18.7 cm2/Vs for ZrOx-based In2O3 TFTs utilizing single and double-layer dielectric, respectively. The proposed method is simple and potentially applicable to other metal oxide dielectrics and semiconductors.