This study presents considerable improvements in the electrical characteristics of atomic-layer-deposited 3-nm-thick In2O3 thin-film transistors (TFTs), which were achieved by introducing a 2-nm-thick amorphous Al2O3 interfacial layer to passivate the surface of a polycrystalline HfO2 gate dielectric. The resulting devices exhibited exceptional electrical characteristics, including an ultrahigh field-effect mobility (μFE) of approximately 147.5 ± 16.6 cm2/V s, subthreshold swing of 103.7 ± 9.1 mV/dec, and threshold voltage (VTH) of 0.5 ± 0.1 V. These enhancement-mode devices represent increases of more than threefold in μFE compared to devices without an amorphous passivation layer. This is despite all the fabrication processes being identical, except for the introduction of the Al2O3 interfacial layer. This improvement can be primarily attributed to the reduced electron scattering through suppressed remote Coulomb interactions. Furthermore, the In2O3 TFTs exhibited enhanced operational stability, showing minimal VTH shifts of 0.15 and −0.01 V under positive and negative bias-stress conditions, respectively. The findings of this study emphasize the critical role of the surface passivation of polycrystalline HfO2 dielectrics in improving the electrical performance of ultrathin In2O3 TFTs.