In this study, an amorphous silica reinforced, phosphoric-crosslinked chitosan foam (P-CTS@SixOy) was prepared. The introduction of amorphous silica not only increased the affinity of the adsorbent for uranium, but also improved the stability of the material. The number of active sites of P-CTS@SixOy was increased by the introduction of phosphate groups. The material exhibited excellent uranium adsorption performance with the removal capacity and efficiency of 850.5 mg g−1 and 98.1 %, respectively. After regenerations, the morphology of P-CTS@SixOy still maintained, and the uranium adsorption efficiency remained above 90 %, manifesting the excellent cycle performance of P-CTS@SixOy. In the dynamic adsorption experiment, P-CTS@SixOy successfully concentrated the volume of uranium-containing solution, and exhibited excellent uranium adsorption performance. The analysis of kinetics, isotherms, and thermodynamics manifested that the uranium adsorption behavior of P-CTS@SixOy was a spontaneous, endothermic, monolayer chemical adsorption process. X-ray photoelectron spectroscopy, Scanning Electron Microscope, and Fourier Transform Infrared Spectrometer were used to characterized the P-CTS@SixOy before and after adsorption, which demonstrated that the main interaction mechanism between uranium and P-CTS@SixOy was the complexation. These studies indicated the huge application prospect of P-CTS@SixOy in the treatment of large-scale uranium-containing wastewater.