The aim of this study was to synthetize new porous nanoparticles based on methyltrimethoxysilane coated hydroxyapatite (MTHAp) for lead removal form aqueous solutions.The morphological and compositional analysis of MTHAp were investigated by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR) and scanning electron microscopy (SEM) equipped with an energy dispersive X-ray spectrometer (EDS). Removal experiments of Pb2+ ions were carried out in aqueous solutions with controlled concentration of Pb2+ at a fixed pH value of 3 and 5 respectively. After the removal experiment of Pb2+ ions from solutions, porous hydroxyapatite nanoparticles were transformed into PbMTHAp 3 and PbMTHAp 5 via the adsorption of Pb2+ ions followed by a cation exchange reaction. The X-ray diffraction spectra of PbMTHAp 3 and PbMTHAp 5 revealed that the powders, after removal of the Pb2+ ions, were a mixture of Ca2.5Pb7.5(PO4)6(OH)2, Pb2Ca4(PO4)2(SiO4), and Ca10(PO4)6(OH)2. Our results demonstrate that the porous hydroxyapatite nanoparticles can be used as an adsorbent for removing Pb2+ ions from aqueous solutions.