Batch lignocellulose-g-poly(acrylic acid)/montmorillonite (LNC-g-PAA/MMT) hydrogel nanocomposites were applied as adsorbents. The nanocomposites were characterized by FTIR, XRD, SEM, and TEM. The results showed that montmorillonite (MMT) could react with the monomers and change the structure of polymeric network of the traditional superabsorbent materials, an exfoliated structure was formed in the nanocomposites. The effect of process parameters such as MMT content (wt%), contact time (t), initial concentration of dye solution (C (0)), adsorption temperature (T), and pH value (pH) of the dye solution for the removal of methylene blue (MB) from aqueous solution were also studied. The results showed that the adsorption capacity for MB increased with increasing contact time, initial dye concentration, and pH value, but decreased with increasing MMT content and temperature. The adsorption kinetics were better described by the pseudo-second-order equation, and their adsorption isotherms were better fitted for the langmuir equation. By introducing 20 wt% MMT into LNC-g-PAA polymeric network, the obtaining hydrogel composite showed the high adsorption capacity 1994.38 mg/g and economic advantage for MB. The desorption studies revealed that the composite provided the potential for regeneration and reuse after MB dye adsorption, which implied that the composite could be regarded as a potential adsorbent for cationic dye MB removal in a wastewater treatment process.