The present study aims at evaluating the batch scale potential of cotton shell powder (CSP), Moringa oleifera leaves (ML), and magnetite-assisted composites of Moringa oleifera leaves (MLMC) and cotton shell powder (CSPMC) for the removal of brilliant green dye (BG) from synthetic wastewater. This is the first attempt to combine biosorbents with nanoparticles (NPs) for the removal of BG. The surface properties of ML, CSP, and their composites were characterized with Fourier-transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), and energy-dispersive X-ray (EDX). The impact of dosage of the adsorbents (1-4g/L), initial concentrations of BG (20-320mg/L), pH (6-12), and contact time (15-180min) on BG removal was evaluated. The BG removal was in order of CSPMC > MLMC > CSP > ML (98.8-86.6% > 98.2-82.0% > 92.3-70.7% > 89.0-57.4%) at optimum dosage (2g/L) and pH (8). Moreover, maximum adsorption (252.17mg/g) was obtained with CSPMC. The experimental results showed better fit with Freundlich adsorption isotherm model and kinetic data revealed that sorption followed pseudo-second-order kinetic model. The values of Gibbs free energy and mean free energy of sorption showed that physical adsorption was involved in the removal of BG. FTIR results confirmed that -O-H, -C-OH, =C-H, -C-H, =-CH3, HC ≡ CH, C=C, -C=O, -C-N, and -C-O-C- groups were involved in the removal of BG. The results revealed that application of low-cost biosorbents combined with NPs is very effective and promising for the removal of textile dyes from wastewater.