Mesoporous materials have great potential for environmental and industrial processes, but many applications require the materials to exhibit specific surface chemistry and binding sites. A new approach has been developed so that organized functional monolayers are covalently bound to mesoporous supports. The functionalized hybrid materials show exceptional selectivity and capacity for removing heavy metals from waste streams. Tailored hybrid materials have also shown potential to selectively bind anions and radionuclides. Rational design of the surface properties of mesoporous materials will lead to more sophisticated functional composites.