The objective of the work described in this thesis was to understand sorption reactions of uranium occurring at the water-clay mineral interfaces in the presence and absence of arsenic and other inorganic ligands. Uranium(VI) removal by clay minerals is influenced by a large number of factors including: type of clay mineral, pH, ionic strength, partial pressure of CO2, load of the sorbent, total amount of U present, and the presence of arsenate and other inorganic ligands such as sulfate, carbonate, and phosphate. Both sulfate and carbonate reduced uranium sorption onto IBECO bentonite due to the competition between SO42- or CO32- ions and the uranyl ion for sorption sites, or the formation of uranyl-sulfate or uranyl-carbonate complexes. Phosphate is a successful ligand to promote U(VI) removal from the aqueous solution through formation of ternary surface complexes with a surface site of bentonite. In terms of the type of clay mineral used, KGa-1b and KGa-2 kaolinites showed much greater uranium sorption than the other clay minerals (STx-1b, SWy-2, and IBECO montmorillonites) due to more aluminol sites available, which have higher affinity toward uranium than silanol sites. Sorption of uranium on montmorillonites showed a distinct dependency on sodium concentrations because of the effective competition between uranyl and sodium ions, whereas less significant differences in sorption were found for kaolinite. A multisite layer surface complexation model was able to account for U uptake on different clay minerals under a wide range of experimental conditions. The model involved eight surface reactions binding to aluminol and silanol edge sites of montmorillonite and to aluminol and titanol surface sites of kaolinite, respectively. The sorption constants were determined from the experimental data by using the parameter estimation code PEST together with PHREEQC. The PEST- PHREEQC approach indicated an extremely powerful tool compared to FITEQL. In column experiments, U(VI) was also significantly retarded due to adsorptive interaction with the porous media, requiring hundreds of pore volumes to achieve breakthrough. Concerning the U(VI) desorption, columns packed with STx-1b and SWy-2 exhibited irreversible sorption, whereas columns packed with KGa-1b and KGa-2 demonstrated slow, but complete desorption. Furthermore, most phenomena observed in batch experiments were recognized in the column experiments, too. The affinity of uranium to clay minerals was higher than that of arsenate. In systems containing uranium and arsenate, the period required to achieve the breakthrough in all columns was significantly longer when the solution was adjusted to pH 6, due to the formation of the uranyl-arsenate complex. In contrast, when pH was adjusted to 3, competitive sorption for U(VI) and As(V) accelerated the breakthrough for both elements. Finally, experiments without sorbing material conducted for higher concentrations of uranium and arsenic showed no loss of total arsenic and uranium in non-filtered samples. In contrast, significant loss was observed after filtration probably indicating the precipitation of a U/As 1:1 phase.