The novelty of the current article is to investigate the adsorption potential of the Egyptian natural and activated bentonite (Na-bentonite) to inorganic and organic phosphorus (IP, OP) in aqueous media. The natural bentonite (NB) was activated to Na-bentonite (Na-B) by a new facile method within 2 h. NB and Na-B were also characterized using XRD, XRF, BET ESM, and FT-IR. The batch experiment has been employed to select the ideal conditions for the removal of inorganic and organic phosphorus (IP, OP) from aqueous solutions. The findings clearly showed that the Na-bentonite is enriched with sodium in the form of Na-montmorillonite with a higher specific area 138.51 m2/g than the value for the natural bentonite 74.21 m2/g. The batch experiment showed maximum absorption for both IP and OP adsorbents occurred at an equilibrium pH = 6, contact time of 40 to 50 min, 40 °C temperature, and a dose rate of 2 mg/L and 1 mg/L, respectively. The equilibrium data displayed better adjustment to Langmuir than the Freundlich, Temkin, and Dubinin-Radushkevich isotherms and adsorption kinetics followed the pseudo-second-order-type kinetic, and the parameters of thermodynamics reveal that adsorption occurs spontaneously and exothermic nature. Na-bentonite proved to be more efficient in removing target material than natural bentonite. The spent bentonites were easily regenerated by chemical methods.