The adsorption of uranyl on two types of neutral (001) surfaces of kaolinite, tetrahedral Si(t) and octahedral Al(o), was studied by means of density functional periodic slab model calculations. Various types of model surface complexes, adsorbed at different sites, were optimized and adsorption energies were estimated. As expected, the Si(t) surface was found to be less reactive than the Al(o) surface. At the neutral Al(o) surface, only adsorption at protonated sites is calculated to be exothermic for inner- as well as outer-sphere adsorption complexes, with monodentate coordination being preferred. Adsorption energies as well as structural features of the adsorption complexes are mainly determined by the number of deprotonated surface hydroxyl groups involved. Outer-sphere complexes on both surfaces exhibit a shorter U-O bond to the aqua ligand of uranyl that is in direct contact with the surface than to the other aqua ligands. This splitting of the shell of equatorial U-O bonds is at variance with common expectations for outer-sphere surface complexes of uranyl.