This dataset includes a set of trajectories from AIMD for models of amorphous alumina at different quenching temperatures, densities and quenching rates. Using the methods described in the associated paper published in Chemical Science, a selection of these confgurations are used to calculated NMR, XAS, and electronic DOS for amorphous alumina. In the associated paper, these spectra are then compared to high-quality experimental results which show excellent agreement with the DFT-computed spectra. All AIMD trajectories were generated using VASP and the subsequent spectroscopic analysis was all carried out using CASTEP. The post-processing tool OptaDOS was then used to generate the XAS spectra and broadened eDOS.