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Here, synthesis of an efficient nanocomposite based on a polyacrylamide grafted carboxymethyl tamarind (CMT-g-PAM) and a SiO₂ nanoparticle is presented. The synthesized nanocomposites are characterized using FT-IR, SEM, TEM, ¹³C NMR, elemental analysis, viscosity, rheological measurement, and molecular weight determination. Various characterizations reveal the existence of an excellent polymer matrix–nanoparticle interaction, which is at a maximum when 1.5 wt % of SiO₂ is introduced in the polymer matrix (i.e., CMT-g-PAM/SiO₂-3). Nanocomposites show tremendous methylene blue (MB) dye adsorption capacity, because of their higher hydrodynamic radius as well as hydrodynamic volume, which originates from proper polymer matrix–SiO₂ nanoparticle interaction. CMT-g-PAM/SiO₂-3 exhibited a maximum adsorption capacity (Q_max) of 43.859 mg·g^–1. The adsorption behavior of the …