The graft copolymerization of acrylic acid (AA) onto starch was carried out with monomer/starch weight ratio 5 1.5. Cerium ammonium nitrate (CAN) and N,N 0 -methylenebis acrylamide (NMBA) were used as initiator and crosslink agent, respectively. Na-montmorillonite was used as nanoparticles. Starch-graft-acrylic acid/Na-MMT (S-g-AA/MMT) nanocomposite hydrogels were characterized by X-ray diffraction (XRD) and FTIR analysis. The effect of Na-MMT content in nanocomposite hydrogels on the swelling behavior was investigated. Increasing the Na-MMT/monomers ratio up to 1% causes an increment in water absorbency, which indicates that Na-MMT can improve the ability of water absorbency but further increase of Na-MMT causes a decrease in water absorbency. In addition, we describe the removal of safranine T from aqueous solutions using S-g-AA/MMT nanocomposite hydrogels. Effects of various parameters such as treatment time, initial dye concentration, and amount of the Na-MMT were investigated. The Freundlich equations were used to fit the equilibrium isotherms.