Ultrahigh-resolution displays for augmented reality (AR) and virtual reality (VR) applications require a novel architecture and process. Atomic-layer deposition (ALD) enables the facile fabrication of indium-gallium zinc oxide (IGZO) thin-film transistors (TFTs) on a substrate with a nonplanar surface due to its excellent step coverage and accurate thickness control. Here, we report all-ALD-derived TFTs using IGZO and HfO2 as the channel layer and gate insulator, respectively. A bilayer IGZO channel structure consisting of a 10 nm base layer (In0.52Ga0.29Zn0.19O) with good stability and a 3 nm boost layer (In0.82Ga0.08Zn0.10O) with extremely high mobility was designed based on a cation combinatorial study of the ALD-derived IGZO system. Reducing the thickness of the HfO2 dielectric film by the ALD process offers high areal capacitance in field-effect transistors, which allows low-voltage drivability and enhanced carrier transport. The intrinsic inferior stability of the HfO2 gate insulator was effectively mitigated by the insertion of an ALD-derived 4 nm Al2O3 interfacial layer between HfO2 and the IGZO film. The optimized bilayer IGZO TFTs with HfO2-based gate insulators exhibited excellent performances with a high field-effect mobility of 74.0 ± 0.91 cm2/(V s), a low subthreshold swing of 0.13 ± 0.01 V/dec, a threshold voltage of 0.20 ± 0.24 V, and an ION/OFF of ∼3.2 × 108 in a low-operation-voltage (≤2 V) range. This promising result was due to the synergic effects of a bilayer IGZO channel and HfO2-based gate insulator with a high permittivity, which were mainly attributed to the effective carrier confinement in the boost layer with high mobility, low free carrier density of the base layer with a low VO concentration, and HfO2-induced high effective capacitance.