The paper considers the importance of nanostructural elements for the creation of multifunctional sorbents. It is known that silicon oxides can be used as nanostructural elements of complex sorbents. The mechanism of absorption of cations of various nature by nanoparticles of polysilicic acids and the features of their coagulation by a nanomagnetite are considered. The use of iron oxides/hydroxides makes it possible to significantly improve the properties of silicon-containing sorbents. Modification of nanoparticles of iron oxides/hydroxides, including iron oxide nanotubes, allows to significantly expand the scope of their application, however, the complexity of manufacturing iron oxide nanotubes is a significant obstacle for practical application. A method of obtaining a multifunctional sorbent based on natural aluminosilicate nanotubes modified with iron (III) hydroxide and ferrocyanide transition metals (in the form of an aqueous dispersion and in a dry state) is proposed, which allows for the purification of radioactively contaminated water from radiocesium with an efficiency of at least 99%. The dispersed composition of the sorbent excludes the possibility of its use in continuous flow conditions. A method of obtaining a granular sorbent has been developed - granules are made from a palygorskite-containing charge by the method of granulation, which, after stepwise heat treatment, are treated with iron (III) hydroxide colloid, followed by the deposition of micro- and nanocrystals of transition metal ferrocyanides on their surface. The resulting mineral composite granulated sorbent is characterized by water resistance and high adsorption properties for ions of alkaline, alkaline earth and transition metals in the presence of organic substances, which allows it to be used in dynamic conditions (filtration through a column) for the treatment of radioactively contaminated waters, in particular, nuclear power plant effluents.