Poly(amidoamine)-graft-poly(methyl acrylate) magnetic nanocomposite was synthesized via radical polymerization of methyl acrylate onto modified magnetic nanoparticles followed by the functionalization of the methyl ester groups with poly(amidoamine) dendrimer. The resulting poly(amidoamine)-graft-poly(methyl acrylate) magnetic nanocomposite was then characterized by infrared spectroscopy, transmission electron microscopy, thermogravimetric analysis, scanning electron microscope and X-ray diffraction analysis. Its application as an adsorbent for the removal of Pb(II) ions was studied. The removal capability of the adsorbent was investigated in different pH values, contact time (kinetics) and initial concentration of lead. Moreover, adsorption isotherms were investigated to describe the mechanistic feature of this nanocomposite for adsorption. Accordingly, its high adsorption capacity (310 mg/g) and efficient adsorption toward lead ions in aqueous solution were shown. To further study of the chemistry behind the adsorption process, a comprehensive density functional theory-based study was performed, and a relatively strong interaction between metal ions and adsorbent was observed based on the calculated adsorption free energies.