Smart core-shell microspheres for selective Pb(2+) adsorption and separation have been developed. Each microsphere is composed of a Pb(2+) recognizable poly(N-isopropylacrylamide-co-benzo-18-crown-6-acrylamide) (PNB) shell and a magnetic Fe3O4 core. The magnetic PNB core-shell microspheres show excellent Pb(2+) adsorption selectivity among the coexisting Cd(2+), Co(2+), Cr(3+), Cu(2+), Ni(2+), Zn(2+), K(+), and Ca(2+) ions by forming stable B18C6Am/Pb(2+) host-guest complexes and exhibit an interesting temperature-dependent Pb(2+) adsorption. The inner independent magnetic Fe3O4 cores enable the Pb(2+)-adsorbed microspheres with a magnetically guided aggregation to be separated from the treated solution using a remotely controlled manner. The isothermal Pb(2+) adsorption result fits well with the Freundlich isotherm. The magnetic PNB core-shell microspheres show very fast adsorption of Pb(2+), and the adsorption process of Pb(2+) onto magnetic PNB core-shell microspheres fits well with the pseudo-second-order model. Moreover, Pb(2+)-adsorbed microspheres can be regenerated by simply increasing the operation temperature and washing with deionized water. The proposed magnetic PNB core-shell microspheres provide a promising candidate for Pb(2+) adsorbents with selectively separable and efficiently reusable abilities.