Amorphous uranium dioxide (UO2) has been modelled on the atomic scale using a combination of quantum mechanical (density functional theory) and classical forcefield methods (molecular dynamics and reverse Monte-Carlo). The atomic scale structure of the amorphous state has been predicted and is presented in the form of simulated X-ray diffraction patterns, pair correlation functions and bond angle distributions. These are shown to be consistent with the experimental patterns previously reported. To enable accurate calculation of the energies and magnetic properties, using quantum mechanics, reverse Monte-Carlo was used to generate reduced cells from larger molecular dynamic melt-quenches. This allowed density functional theory energy minimisation for structures consistent with the amorphous state. Building on this, the material's propensity to deviate from stoichiometry, the magnetic structure and amorphous UO2 surface energy were computed. Non-stoichiometry is accommodated more readily in the amorphous system than in crystalline UO2. This indicates that deviations from stoichiometry in fuel (for example as a result of operation) will be accommodated at amorphous phases, if present, leaving a more stoichiometric bulk phase – impacting processes including fission gas mobility, melting points and a number of other safety relevant properties. The magnetic structure of bulk amorphous UO2 is predicted to be a spin-glass, unlike crystalline UO2 which has anti-ferromagnetic ordering at 0 K. The surface energy of amorphous UO2 is computed to be 0.79 Jm−2, which is similar to the experimentally observed surface energy of grain boundary bubbles in UO2 and comparable to the surface energies reported for crystalline UO2. Results are pertinent to ongoing efforts to understand the nature of grain boundaries in nuclear fuels, to model fission gas release from them, radiation induced amorphization and the impact of dopants and impurities on nuclear fuel's manufacture and in-reactor behaviour.