A series of copolymeric hydrogels comprising of acrylic acid and acrylamide and crosslinked with trimethylolpropane triacrylate (TMPTA) were prepared using ammonium persulfate (APS) as initiator. The hydrogels were functionalized further by partial hydrolysis and were characterized by SEM, FTIR, nitrogen analysis, and also by water uptake studies as a function of time, temperature, pH, NaCl, and concentration of sodium dodecyl sulfate (SDS). These hydrogels were used as sorbents for the uranyl ions uptake in the presence of 5% NaCl, which was studied as function of time, temperature, pH, and ion strength. The uranyl uptake was found to be affected both by the structural aspects of the hydrogels as well as by the external environmental factors.