Natural pyrite was modified by calcination under nitrogeni (N2) atmosphere to produce a novel sorbent for removing phosphorus (P) with low concentration from aqueous solutions. The crystallinity, porous texture, magnetic susceptibility, and performance in P removal of pyrite calcinates depended on calcination temperatures. The sorbent obtained at calcination temperature of 500 - 600 oC possessed the most efficient P removal. Solution pH in the range of 3.0 - 9.0 and anions of chloridion (Cl-), nitrate (NO3)- and sulfate (SO42-) had ignorable effect on P removal. The batch adsorption experiment shows that the maximum sorption capacities for P of this novel sorbent (qm) was up to 1.61 - 5.36 mg P/g at adsorption temperatures of 15 - 35 oC. Dynamic sorption and regeneration experiments were conducted in an adsorption column filled with pyrite calcined at 600 oC. The study found that oxygen was an important control factor responsible for P adsorption because the oxidization of Fe2+ to Fe3+ on the surface of the sorbent followed by P being bound to a ferric hydroxide surface film were the crucial processes. The mechanism was confirmed with surface characterization techniques including field emission scanning electron microscope (FE-SEM) and X-ray photoelectron spectroscopy (XPS). This research potentially provides a cheap, abundant sorbent for P removal from the secondary effluent of municipal wastewater treatment plant.