A novel modification through pressurized filtration technique of commercial polyethersulfone membranes was proposed using a biopolymer extracted from Moringa oleifera Lam. (MO) along with graphene oxide (GO), in order to decrease fouling and improve the membrane selectivity for the removal of methylene blue dye. The effect of these agents over the morphology and performance of the membranes were studied through the evaluation of permeability, dye removal and fouling parameters. The characterization of the membrane indicates a significant decrease in pore size, as confirmed by the filtration experiments. Also, according to FTIR and SEM analysis the modification was effectively accomplished. All modified membranes presented low fouling rates (<10.55%) and high dye removal rates (from 2.85% to 96.73%). Furthermore, it is the first time that MO has been used as a natural polymer to improve and confer new characteristics on membranes, creating new possibilities for further study of this promising environment-friendly biopolymer in membrane separation processes.