Sediments from aquatic environments can be contaminated with uranium from natural and anthropogenic sources; the behavior of U(VI) was investigated in two natural (SPT and DS) and gamma-irradiated (SPT-I) aquifer sediments in batch systems. Sediments were characterized, and quartz, albite, and kaolinite were mainly found in both sediments by X-ray diffraction. The points of zero charge were 5.4, 5.3, and 5.5, and the organic matter percentages were 48.0, 46.0, and 4.7% for SPT, SPT-I, and DS, respectively. Uranyl nitrate solutions were put in contact with each sediment considering different parameters (pH, contact time, initial concentration of uranium, and temperature). DS sediment did not adsorb any quantity of uranium at different pH values; SPT and SPT-I, attained the highest q e values at pH 3.5–4. The results show chemisorption on homogenous materials and endothermic processes. Desorption behavior of U(VI)/SPT showed a hundred percent desorption with nitric acid and humic acid solutions; in the last case, it is due to the high stability constant of the complex of uranium with the humic acids. The results help to understand the contamination and decontamination processes of sediments with uranium, the bioavailability of uranium, the ecological risk of U-contaminated sediments, and remediation. Doses of 1 MGy of Co-60 gamma radiation did not affect the uranyl ions behavior in the aquifer sediment.