Palm shell-based adsorbents prepared under five different thermochemical conditions and palm shell powder have been shown to be quite effective for removal of uranium from aqueous solutions. X-ray photoelectron spectroscopy (XPS), extended X-ray absorption fine structure (EXAFS), and Fourier transform infrared spectroscopy (FTIR) have been used to determine information about the speciation and binding of uranium on the adsorbents under study. Studies indicate that the uranium which is present as uranyl ion in aqueous solution is present in mixed valence states (U(IV), U(V), and U(VI)) when it is bound to the adsorbents. The mechanism of adsorption is likely to be adsorption-coupled reduction as well as complexation. Adsorption of uranium, cesium, and iron was found to be quantitative in binary as well as ternary mixtures.