<p>Mechanical properties of ultrathin coatings can deviate from bulk values due to growth-stage and interface effects. Elastic moduli of bulk amorphous alumina were calculated using a near-ab initio-accurate neural-network interatomic potential to provide a modeling benchmark for hydroxylated alumina coatings deposited by atomic layer deposition at 50 °C. Experimentally, elastic moduli were evaluated by both spherical nanoindentation and laser-induced surface acoustic wave spectroscopy (LiSAWS). For coatings thicker than 7 nm, both techniques indicated a weakly decreasing modulus from ~137 GPa to ~126 GPa (nanoindentation) and ~116 GPa to ~108 GPa (LiSAWS). These values are consistent with the simulated Young’s modulus.</p>