Leaching experiments with metallic uranium-aluminum research-reactor fuel elements in repository-relevant MgCl2-rich salt brine (brine 2) were performed. A Mg-Al layered double hydroxide (LDH) with chloride as the interlayer anion was identified as a crystalline secondary-phase component. In the present study, the incorporation of Cd into the structure of the Mg-Al-Cl LDH was investigated. Synthesis by a coprecipitation method was performed and the Mg-Cd-Al-Cl LDH obtained was characterized. The sorption behavior of selenium on the LDH was investigated in water, clay pore-water (Mont-Terri-type), and brine 2. Using a LDH concentration of 10 g/L, the sorption kinetics were rapid and equilibrium was reached within 12 h. The sorption of selenium decreased with increasing amount of chloride anions in the solutions. The chloride anions acted as competing anions for the sorption of selenium. The effect of pH on selenium sorption was investigated and a large buffer capacity of the LDH was observed. For the range of selenium concentration used, linear sorption isotherms were obtained which obeyed the Freundlich and Dubinin-Radushkevich models. From these, the energies of selenium sorption were calculated to be in the range of ion-exchange processes.