Hybrid materials with organic-inorganic character have been receiving attention especially due to their unique properties and offer probability for many new applications in variable fields and industrial applications. One of these applications is heavy metal removal from aqueous solutions because the metal pollution is a matter of concern about environment. In this study, organic-inorganic hybrid materials on the basis of metal alkoxides and their calcined forms were synthesized, characterized, and applied firstly to remove Cu(II), Fe(III), Pb(II), and Zn(II) ions from aqueous solutions by adsorption process. Response surface methodology was applied to optimize metal ions removal.