Oxide semiconductor based thin-fi lm transistors (TFTs) are a promising technology for application in large-area electronics. [ 1 ] Despite their relatively short history, oxide TFTs with chargecarrier mobilities exceeding 100 cm 2 V − 1 s − 1 [ 2,3 ] have already been demonstrated, a performance that is superior to that of amorphous silicon (a-Si) and comparable to polycrystalline Si (poly-Si). Unfortunately, these high-mobility oxide TFTs are usually manufactured using costly vacuum-based processing methodologies. [ 1 , 4-8 ] In an effort to address this problem, recent research has been focussing on the development of TFTs using alternative deposition methods based on solution-processable oxide semiconductors. [ 9 -14 ] Whilst progress on solution-processed oxide semiconductors has been rapidly advancing, research efforts towards the development of new dielectrics has been relatively slow, with most of the reported work performed using conventional dielectrics (e.g., SiO 2 ) with few exceptions. [ 9 , 15,16 ] As a result, the majority of oxide transistors reported to date operate at relatively high voltages and hence consume signifi cantly more power. In order to circumvent this bottleneck, recent work has been focusing on the development of low-voltage oxide transistors, including the use of ultra-thin dielectrics, [ 17 ] high -k dielectrics, [ 15 ] and electrolyte gate dielectrics. [ 18 ] Oxide transistors based on high -k dielectrics have received the most attention and a number of high mobility, low-voltage devices have been demonstrated. [ 15 , 17 ] The high -k materials studied to date include transition metal oxides such as Ta 2 O 5 , TiO 2 , [19][20][21][22] ZrO 2 , [23][24][25][26] Al 2 O 3 , [ 27 ] HfO 2 , [ 28 ] and silicates, [ 29 ] as well as ferroelectric materials such as Pb(Zr,Ti) O 3 and (Ba,Sr)TiO 3 . [ 30 , 31 ] Among these, ZrO 2 and HfO 2 are the most extensively studied dielectrics and are widely considered to be excellent candidates because of their relatively high dielectric constants, good thermal stability, and large band gaps. [32][33][34] Despite their attractive properties, however, ZrO 2 and HfO 2 based TFTs are usually realised using stringent and potentially costly manufacturing techniques. [35][36][37][38][39] Here we demonstrate how spray pyrolysis (SP), a simple and large-area-compatible deposition technique, can be used for the processing of high-quality ZrO 2 layers onto glass substrates containing prepatterned indium tin oxide (ITO) electrodes. We demonstrate their use in high-mobility, low-voltage TFTs based on either ZnO or Li-doped ZnO fi lms deposited by SP [10][11][12][13][14] directly onto ITO/ZrO 2 . Optimised TFTs based on ITO/ZrO 2 / Li-ZnO multilayer structures deposited sequentially at substrate temperatures of 400-450 ° C exhibit excellent electrontransport characteristics with operating voltages below 6 V and a maximum electron mobility on the order of 85 cm 2 V − 1 s − 1 . To our knowledge, this is the highest reported mobility value for transistors bas...