Hydrogel nanocomposites having high amount of functional group, enhanced swelling ability, and improved mechanical properties were prepared for removal of basic dyes from aqueous solutions. Acrylamide (AAM) and itaconic acid sodium salt (IANa) were polymerized using polyethyleneglycol (400) diacrylate as crosslinker in the presence of montmorillonite (MMT). The products were characterized by swelling degree, total basic group content, XRD analysis, and FTIR spectroscopy. It was observed that MMT addition increased the itaconic acid gelation. The incorporation of low amount of MMT into the hydrogel structure increased also swelling degree. The products were used as adsorbent for removal of brilliant cresyl blue (BCB) from aqueous solutions. It was observed that the adsorption of BCB onto the nanocomposite completed in 30 min. It was found that the adsorption kinetics followed a pseudo-second-order kinetic model. Equilibrium isotherm of nanocomposite was analyzed using Freundlich and Langmuir isotherms. It was seen that the Langmuir isotherm model fit the adsorption data. These hydrogel nanocomposites have been shown to have the potential to be used as novel, fast-responsive and high capacity adsorbent materials for the removal of cationic dyes which is a serious problem, especially in textile industry.