Low-temperature atomic layer deposition (ALD) was employed to deposit Al2O3 as a gate dielectric in amorphous In-Ga-Zn-O thin-film transistors fabricated at temperatures below 120 °C. The devices exhibited a negligible threshold voltage shift (ΔVT) during negative bias stress, but a more pronounced ΔVT under positive bias stress with a characteristic turnaround behavior from a positive ΔVT to a negative ΔVT. This abnormal positive bias instability is explained using a two-process model, including both electron trapping and hydrogen release and migration. Electron trapping induces the initial positive ΔVT, which can be fitted using the stretched exponential function. The breakage of residual AlO-H bonds in low-temperature ALD Al2O3 is triggered by the energetic channel electrons. The hydrogen atoms then diffuse toward the In-Ga-Zn-O channel and induce the negative ΔVT through electron doping with power-law time dependence. A rapid partial recovery of the negative ΔVT after stress is also observed during relaxation.