In this article, we report the mechanism and kinetics of adsorption of uranyl ions on starch-based functional hydrogels. The hydrogels were prepared from starch in native or hydrolyzed/oxidized form by crosslinking with N,N-methylenebisacrylamide. The hydrogels synthesized from the oxidized starch have carboxylic groups at C-6 position. The effect of the structure and external environmental factors, i.e., contact time, temperature, ion strength, and simulated seawater (0.55 M NaCl and 3 mM NaHCO3), was investigated on the uranyl adsorption behavior of hydrogels. The adsorption of uranyl ions was rapid as the highest adsorption was observed after 6 h and at 40°C. The sorbents also exhibited appreciable ion uptake even from the simulated seawater. The equilibrium data was analyzed using Langmuir and Freundlich adsorption isotherms and pseudo-first order and pseudo-second order kinetic models. Evidence of adsorption was obtained by characterization of the uranyl ions-loaded hydrogels by FTIR spectroscopy and also by elution with 0.1 N HCl.