A review with ca. 400 references is provided dealing with the use of mesoporous silica and organically-modified silica-based materials for removal of inorganic and organic pollutants from aqueous solutions. After having briefly discussed the interest of functionalized mesoporous silica for environmental remediation purposes, the various synthetic methods to prepare such nanoengineered adsorbents are described. Then, their application to the removal of heavy metal species, toxic anions, radionuclides, and a wide range of organic pollutants is presented in a comprehensive way with the help of extensive tables and some illustrating figures.