In this work, adsorption feasibility of a cationic dye, methylene blue (MB), onto an anionic hydrogel nanocomposite was investigated in detail. Firstly, the hydrogel nanocomposite was synthesized via a simple solution copolymerization of acrylic acid and 2-acrylamido-2-methylpropanesulfonic acid monomers in the presence of montmorillonite (MMT) by using ammonium persulfate as an initiator and methylene bisacrylamide as a crosslinker. Then, the effects of agitation time, MMT content, pH, initial dye concentration, adsorbent dose, and temperature were optimized with respect to the dye adsorption capacity of nanocomposites. The thermodynamic parameters such as changes in standard free energy, enthalpy, and entropy demonstrated that dye adsorption onto the hydrogel nanocomposite was spontaneous and endothermic, and especially more effective at high temperatures. Moreover, the results indicated that the equilibrium adsorption isotherm data of the hydrogel nanocomposite better fit to the Redlich-Peterson than to the Langmuir, Freundlich, and Temkin models. The experimental results also fit to pseudo-first-order, pseudo-second-order, and intraparticle diffusion kinetic models. The results indicated that the adsorption of MB followed pseudo-second-order kinetics.