Composite adsorption materials combine the advantages of various adsorptive materials and compensate for the defects of single adsorbents. Magnetic montmorillonite (MMMT) shows good adsorption properties for Pb(II). In order to further improve the adsorption properties of MMMT, in this work, Zn-BDC, a kind of metal–organic framework (MOF), was modified onto the surface of MMMT by in situ polymerization. The composite material MMMT@Zn-BDC was characterized by Zetasizer, SEM, TEM, FTIR, XRD, VSM, and XPS. The influence of adsorption conditions on the adsorption capacity of MMMT@Zn-BDC for Pb(II) was examined, including the adsorbent dosage, pH of Pb(II) solution, initial concentration of Pb(II), and the temperature and adsorption time. Also, the adsorption mechanism was studied. The results of this study show that MMMT@Zn-BDC adsorbs Pb(II) via chemisorption. In addition, MMMT@Zn-BDC exhibits good potential for adsorbing Pb(II), including its high adsorption capacity (724.64 mg/g) and good recyclability.