The impregnation of titania causes to generate and activate more points on surface of bentonite which is usually slightly basic in nature. That helps in the removal of cationic impurities effectively. So, their composite (TBC) is prepared and used to remove brilliant green (BG) dye as a test case here in cost-effective and ecofriendly manner by green methodology. The surface modification was analyzed by FTIR and SEM/EDX. Adsorption parameters were investigated and found that 4.54 mg/g ± 0.73 S.D of dye was removed by this composite using optimized condition. In kinetic study, pseudo-second order model justified the data. Thermodynamic value is −10.33 kJ/mol ± 0.067 indicating its exothermic and spontaneous nature of process. Desorption of BG and regeneration of titania–bentonite composite with HCl helps in its recycling and affirms that these nanocomposites are prolific, high-yielding and resourceful material for dye removal during wastewater treatment.