Mesoporous metal-organic framework-5 (MOF-5), with the composition Zn4O(BDC)3, showed a high capacity for the adsorptive removal of Pb(II) from 100% aqueous media. After the adsorption process, changes in both morphology and composition were detected using a scanning electron microscope (SEM) equipped with an energy dispersive X-ray (EDX) system, Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS) analysis. The experimental evidence showed that Zn(II) liberation from MOF-5 structure was provoked by the water effect demonstrating that Pb(II) removal is not due to ionic exchange with Zn. A kinetic study showed that Pb(II) removal was carried out in 30 min with a behavior of pseudo-second-order kinetic model. The experimental data on Pb(II) adsorption were adequately fit by both the Langmuir and BET isotherm models with maximum adsorption capacities of 658.5 and 412.7 mg/g, respectively, at pH 5 and 45°C. The results of this work demonstrate that the use of MOF-5 has great potential for applications in environmental protection, especially regarding the removal of the lead present in industrial wastewaters and tap waters.