Selective adsorption of Pb(II) and Cr(VI) by surfactant-modified and unmodified zeolites is discussed in this paper. The influences of pH, ionic strength, temperature, and adsorption time on Cr(VI) and Pb(II) adsorption are studied, The characteristics of the surface and inner structures of zeolites before and after modification are analyzed through infrared spectroscopy, scanning electron microscopy, X-ray diffraction, Brunauer-Emmett-Teller analysis, and zeta potential measurement. Results show that the characteristics of electric charge on the zeolite surface had changed after modification, which resulted in selective adsorption of Cr(VI) and Pb(II). Moreover, kinetic study reveals that adsorption by the different zeolites coincides with the Langmuir model and pseudo-secondorder kinetic equation. The intraparticle diffusion equation proves that the Cr(VI) adsorption is mainly electrostatic, whereas Pb(II) adsorption proceeds via intrapore and electrostatic adsorption on the zeolite surface. This difference in mechanisms endows selectivity of metal ion adsorption by the modified zeolites. This study provides a reference on zeolite modification for use in various applications, such as wastewater treatment.