Metal organic frameworks (MOFs) have been regarded as robust adsorbents for the adsorptive removal of organic pollutants because of their unique characteristics. However, the application of MOFs in the removal of metals from water is still rare. In this paper, amino-functionalization of Cr-based MOFs MIL-101 are modified through coordination bonding of unsaturated Cr metal centers with the −NH 2 group in ethylenediamine (ED), and we demonstrate their excellent performance for the removal of Pb(II) ions from water. The Fourier transform infrared verifies that the ethylenediamine was grafted successfully on MIL-101. Furthermore, the results of X-ray diffraction, scanning electron microscopy, and transmission electron microscopy show that the structure of ED-MIL-101 with an appropriate amount of ED almost does not collapse and retains the original performance of MIL-101. The adsorption capacity of ED-MIL-101, which is more than five times that of MIL-101, is 81.09 mg·g −1 for Pb(II) ions from aqueous samples. The selectivity coefficients of ED-MIL-101 for Pb(II)/Cu(II), Pb(II)/ Zn(II), Pb(II)/Co(II), and Pb(II)/Ni(II) are 6.92, 24.02, 15.69, and 14.53, respectively. The adsorption kinetics of Pb(II) ions shows that the process fits well with a pseudo-second-order model, and the adsorption equilibrium time is only about 30 min. Moreover, the practical application of ED-MIL-101 achieves almost 97.22% removal efficiency for Pb(II) ions. These results indicate that ED-MIL-101 has great potential in selectively removing Pb(II) ions from water environment.