Interaction of aqueous UO22+ solutions with modified sorbents based on coarsely porous silica gel MSKG, containing Cu, Ni, and Zn ions, was studied. Uranyl ions are sorbed on all the sorbents. The decontamination factors of 10−2 M aqueous UO22+ solutions on straight MSKG and on MSKG modified with Cu, Ni, and Zn are of the same order of magnitude and do not exceed 100. In the case of 1.1 × 10−1 M UO22+ solutions, the decontamination factors on straight MSKG and on MSKG modified with Cu, Ni, and Zn are also of the same order of magnitude but do not exceed 10. Interaction of the modified Ni-containing sorbent with a UO22+ solution results in formation of a swamp-green precipitate of the composition NiU(OH)6•4N2H5OH, i.e., UO22+ is reduced to U4+.