Al2O3 has emerged as the surface passivation material of choice for p-type silicon in photovoltaics and has also become a candidate for passivating Si-based radiation sensors. However, the surface passivation of Al2O3 has been shown to degrade when exposed to gamma-radiation, making it of interest to determine methods of depositing Al2O3 that minimize the radiation-induced degradation on the surface passivation. In this study, we investigate the long-term stability and gamma-radiation hardness of Al2O3 prepared using the TMA+H2O+O3 precursor combination and how the pretreatment, the deposition temperature, and the film thickness affect the density of interface states, Dit, and fixed oxide charge, Qfix, before and after gamma-irradiation. We find that the surface saturation current density, J0s, of silicon passivated by Al2O3 increases after annealing but stabilizes over time depending on the Al2O3 thickness. Samples with thicknesses of <20 nm stabilize within hours, while those with >60 nm stabilize over days. J0s stabilizes at lower values with increased Al2O3 thickness. After exposure to 1 Mrad gamma-radiation, the samples still exhibit low Dit and high Qfix, with the best performing sample having a Dit of 1.5 × 1010 eV−1 cm−2 and a Qfix of −3.1 × 1012 cm−2. The deposition temperature appears to indirectly affect radiation hardness, owing to its impact on the hydrogen concentration in the film and at the Si–SiOx–Al2O3 interface. Lifetime measurements after irradiation indicate that Al2O3 still passivates the surface effectively. The carrier lifetime and Qfix can largely be recovered by annealing samples in O2 at 435 °C.