Anthropogenic activities have led to an increased concentration of uranium on the Earth's surface and potentially in the subsurface with the development of nuclear waste repositories. Uranium is soluble in groundwater, and its mobility is strongly affected by the presence of clay minerals in soils and in subsurface sediments. We use molecular dynamics simulations to probe the adsorption of aqueous uranyl () ions onto the basal surface of muscovite, a suitable proxy for typically ultrafine-grained clay phases. Model systems include the competitive adsorption between potassium counterions and aqueous ions (0.1 M and 1.0 M UO2Cl2, 0.1 M NaCl). We find that for systems with the presence of potassium and uranyl ions, potassium ions dominate the adsorption phenomenon. Potassium ions adsorb entirely as inner sphere complexes associated with the ditrigonal cavity of the basal surface. Uranyl ions adsorb in two configurations when it is the only ion species present, and in a single configuration in the presence of potassium. The majority of adsorbed uranyl ions are tilted < 45° relative to the muscovite surface, and are associated with the Si4Al2 rings near the aluminium substitution sites.