The simultaneous removal of phosphate and aluminum from water was studied on iron-modified activated carbons. Methods such as oxidation with HNO3, impregnation and co-precipitation of iron were used to modify a commercial coconut activated carbon and to obtain seven different modified carbons. The physicochemical properties of selected samples were studied by different analytic methods such as FT-IR spectroscopy, SEM/EDX analysis and X-ray diffraction. Adsorption studies of phosphate and aluminum from water in single and binary systems were performed in bath systems with constant agitation at 30 °C and different values of pH. Particularly, the sample obtained by Oxidation-Impregnation-Drying procedure (CCOFeTB) contains 3.80% of iron in amorphous phase according to the EDX and XRD analysis, respectively. Additionally, this sample showed the best adsorption performance achieving an adsorbed amount of phosphates of 23.33 mg/g at pH 2 in single system. In binary systems, it was observed a synergistic effect in the adsorption of both species (phosphate and aluminum) and the principal adsorption mechanism is related to electrostatic interactions according with the results of molecular simulation.