In developing low-power electronics, low-voltage transistors have been intensively investigated. One of the most important findings is that some high-k oxide gate dielectrics can lead to remarkable enhancement of apparent mobility in thin-film transistors (TFTs), which is not clearly understood. Here, we investigate InO x TFTs with solution-processed AlO x dielectrics. At very low frequencies (<1 Hz), the AlO x films feature strong voltage-dependent capacitance. Also, cyclic voltammograms show clear features of surface-controlled Faradaic charge transfer. The two independent experiments both point to the formation of pseudocapacitance, which is similar to the mechanism behind some supercapacitors. A physical model including charge transfer is established to describe ion distribution. The charge transfer is probably related to residual hydrogens, as revealed by secondary-ion mass spectroscopy. The results provide direct evidence of the formation of pseudocapacitance in TFTs with high apparent mobilities and advance the understanding of mechanisms, measurements, and applications of such TFTs for low-power electronics.M etal-oxide thin-film transistors (TFTs) have attracted significant attention for applications in the area of active-matrix devices such as high-resolution displays with organic light-emitting diodes. 1−4 The advantages include largearea uniformity, high mobility, and compatibility in a flexible electronic device. To improve the performance of the metaloxide TFTs, high-k dielectrics have been used as gate insulator in metal-oxide TFTs such as Y 2 O 3 , Al 2 O 3 , ZrO 2 , and HfO 2 . 5−8 It is exciting to note that there are considerable reports that the solution-processed high-k gate dielectric induces remarkable enhancement of mobility, 9,10 with several to 10 times as compared with that in the cases with thermal silicon oxide gate. However, no consensus yet exists on how to explain this remarkable enhancement.Lee et al. attributed the mobility enhancement to the increased capacitance and carrier density using a high-k gate dielectric. 11 However, for some TFTs with high-k gate dielectrics, the mobility was not enhanced. 6,12 Zeumault et al. proposed that donor-like traps in ZrO 2 are aligned at shallow energies with respect to the transport band of ZnO and provide more carriers in the ZnO channel by charge migration at the insulator/semiconductor interface, resulting in high mobility. 13 Heo et al. attributed the mobility enhancement to electric double layer (EDL) formation at the solutionprocessed AlO x /InO x interface. 14 In most cases, large capacitance induced by EDL can lead to low operating voltage. However, numerical simulations have revealed that, once the