The presence of dyes in water stream is a major environmental problem that affects aquatic and human life negatively. Therefore, it is essential to remove dye from wastewater before its discharge into the water bodies. In this study, Banyan (Ficus benghalensis, F. benghalensis) tree leaves, a low-cost biosorbent, were used to remove brilliant green (BG), a cationic dye, from an aqueous solution. Batch model experiments were carried out by varying operational parameters, such as initial concentration of dye solution, contact time, adsorbent dose, and pH of the solution, to obtain optimum conditions for removing BG dye. Under optimum conditions, maximum percent removal of 97.3% and adsorption capacity (Qe) value of 19.5 mg/g were achieved (at pH 8, adsorbent dose 0.05 g, dye concentration 50 ppm, and 60 min contact time). The Langmuir and Freundlich adsorption isotherms were applied to the experimental data. The linear fit value, R2 of Freundlich adsorption isotherm, was 0.93, indicating its best fit to our experimental data. A kinetic study was also carried out by implementing the pseudo-first-order and pseudo-second-order kinetic models. The adsorption of BG on the selected biosorbent follows pseudo-second-order kinetics (R2 = 0.99), indicating that transfer of internal and external mass co-occurs. This study surfaces the excellent adsorption capacity of Banyan tree leaves to remove cationic BG dye from aqueous solutions, including tap water, river water, and filtered river water. Therefore, the selected biosorbent is a cost-effective and easily accessible approach for removing toxic dyes from industrial effluents and wastewater.