Two chitosan silica hybrid materials were prepared by a two-step process in 78–84% yields using the homogeneous phase reaction of 3-(triethoxysilyl)propyl isocyanate with chitosan dissolved in 1-n-butyl-3-methylimidazolium chloride ionic liquid (∼10% w/w), which was followed by NH4OH catalyzed hydrolysis of triethoxysilyl groups and then sol-gel process. These new hybrid materials were shown to adsorb up to about 95% of Fe3+ from 5 × 10−4 M aqueous solution at room temperature in 24 h.