Uranium-containing wastewater poses a significant threat to both the ecological environment and human health. Adsorption is a crucial method for purifying uranium wastewater. Using 3-Aminopropyltriethoxysilane (APTES) to modify attapulgite (ATP), we successfully prepared a cost-effective and high-performance adsorbent material, APTES-modified attapulgite (APTES/ATP). This material was utilized for the purification of uranium-containing wastewater. Characterization techniques were employed to study the structure and surface properties of the material. The adsorption performance of the material was investigated using single-factor experiments. The adsorption isotherms, kinetics, and thermodynamics were also studied and discussed. The results indicated that APTES/ATP exhibited an adsorption capacity of 382.13 mg·g−1 for uranium at room temperature. The adsorption process followed the Langmuir adsorption model and pseudo-second-order kinetics, indicating that the adsorption of uranium by the material was a monolayer chemisorption. Adsorption thermodynamics revealed that the process was endothermic and spontaneous. The adsorption mechanism primarily involved electrostatic attraction and interactions between −NH2, Si-O, and −OH groups with uranium. In summary, the prepared APTES/ATP demonstrated excellent adsorption capacity for uranium and shows promise for the purification of uranium-containing wastewater.