An organic–inorganic hybrid mesoporous silica was synthesized via post-grafting of KIT-6 with 4-(triethoxysilyl)butyronitrile. All samples were characterized using their N2 adsorption–desorption isotherms, XRD, FT–IR, TEM, SEM, and PT. The adsorption potential of this material for removing Pb(II) from aqueous solutions was investigated via the batch technique, and the effects of pH and contact time were studied. Experimental data showed that the maximum Pb(II) adsorption, 76%, occurred in the pH range around 6. The adsorption equilibrium was reached within 40min for 10wt.%COOH/KIT-6. The adsorption data were fitted using the Langmuir and Freundlich isotherms, and the obtained modeling equilibrium adsorption data suggested that the 10wt.%COOH/KIT-6 sample contained homogeneous adsorption sites that fit the Langmuir adsorption model well. The pseudo-second-order model described well the 10wt.%COOH/KIT-6 adsorption process. The desorption and regeneration experiments indicated that ≈95% of the metal desorbed and the adsorbent could be regenerated via an acid treatment without altering its properties.