A sources of entering uranium to surface and ground water are some minerals and also anthropogenic factor, particularly military activity that involves projectiles containing depleted uranium. Under elevated temperatures, this metal is oxidized producing U3O8, further oxidation and hydration gives soluble U(VI) compounds. This work is devoted to the development of sorbents for the removal of these toxic contaminants from water. They are based on gel-like strongly acidic resins, to which the nanoparticles of zirconium hydrophosphate (ZHP) were embedded. The amount of additionally sorbed zirconium salt and its concentration were controlled to obtain the composites of different morphology. Particularly the nanocomposite containing only non-aggregated particles (2–10 nm) was obtained. Smaller nanoparticles are formed preferably in rigid polymer. The isotherms of U(VI) sorption were fitted with Langmuir and Dubinin-Radushlevich models. The nanocomposite that is free from aggregates shows an increase of the monolayer capacitance in 1.2–2 times comparing with the pristine resin, a growth of entropy was also detected. The sorption mechanism is ion exchange, the adsorption heat is 56.8 (pristine sample) and 65.9 (nanocomposite) kJ mol−1.