Polyhedral oligomeric silsesquioxane and organosilicon polymers, which are important classes of inorganic-organic hybrid materials, have emerged as effective adsorbents for the removal of contaminants from the wastewater. In this study, two hybrid materials polyhedral oligomeric silsesquioxane (1-(3-(polyhedraloligomericsilsesquioxane)propoxy)ethane-1,2-diol, POSS-diol) and organosilicon polymer (PGPTS) as adsorbents have been synthesized from 3-glycidyloxypropyltrimethoxysilane (GPTS) monomers by using basic catalyst tetrapropylammonium hydroxide (Pr4NOH(aq)) and acidic catalyst chlorotinbis[trimethylsilyl)]amide (SnCl(HMDS)), respectively. These hybrid materials POSS-diol and PGPTS were characterized by a few instrumental techniques such as NMR, FTIR, GPC, XRD, BET and then used in the removal of methylene blue (MB) dye from aqueous solutions. These hybrid silicon materials showed an exceptionally high degree of adsorption for MB dye compared to GPTS hydrolyzed with HCl(aq) (POSS-epoxide) and inorganic-organic hybrid materials of Al, Ti, and Zr. The reason for this high adsorption capacity of MB has been tried to be determined mechanically and discussed.