A series of sorption materials based on layered double hydroxides (Co-Fe LDH, Ni-Fe LDH, and Zn-Ti LDH) were obtained by a facile and environmentally friendly method of coprecipitation. A low particle size of no more than 10 µm was achieved. The use of transition metals makes it possible to obtain compounds that are mechanically and chemically stable in aggressive environments. XRD analysis revealed that the compounds have a highly organized crystalline structure. Using SEM, it was determined that Co-Fe LDH and Ni-Fe LDH had a loose, highly dispersed surface structure, while Zn-Ti LDH had a monolithic surface structure. U(VI) adsorption on the obtained materials in solutions containing Na2CO3, Na2SO4, KNO3, NaCl, K3PO4, and NaHCO3, was studied in batch mode. The degree of purification in the presence of these salts reached 99.9%, while the distribution coefficient Kd reached 105 mL/g. Sorption capacity qmax and equilibrium adsorption constants Kf and KL for U(VI) adsorption in batch mode (for 24 h) from distilled and seawater were determined using the Freundlich and Langmuir equations. The highest sorption capacity of 101.6 mg/g in seawater and 114.1 mg/g in distilled water was registered for Co-Fe-LDH. The presence of competing ions in seawater can reduce sorption efficiency by up to 40%. The provided research allowed us to conclude that the obtained materials, Co-Fe LDH, Ni-Fe LDH, and Zn-Ti LDH are promising for the sorption removal of U(VI) from aqueous media of medium salinity.