Two novel inorganic-organic hybrid materials, Al-Pydca-3-APDEMS-H and Zr-Pydca-3-APDEMS-H, were prepared by the sol gel method in two steps. In the first step, Al((OBu)-Bu-s)(2)-Pydca and Zr(OPrn)(3)-Pydca complexes were prepared from the reactions of aluminum sec-butoxide Al((OBu)-Bu-s)(3) and zirconium n-propoxide Zr(OPrn)(4) with 2,6-pyridinedicarboxylic acid, respectively. After 3 h of stirring, 3-aminopropyldiethoxymethyl silane (3-APDEMS) and dilute hydrochloric acid were added to the Al((OBu)-Bu-s)(2)-Pydca and Zr(OPrn)(3)-Pydca mixtures to hydrolyze the reactions and to form condensation products. These hybrid products were characterized by a combination of Fourier-transform infrared (FT-IR) spectroscopy, powder X-ray diffraction (XRD), scanning electron microscope (SEM), energy-dispersive X-ray (EDX) spectroscopy, Brunauer-Emmett-Teller (BET) analysis, Barrett-Joyner-Halenda (BJH) and other analysis methods. These hybrid materials were used for the removal of methylene blue (MB), a cationic organic dye. The removal efficiency of hybrid materials was measured by UV-Vis spectroscopy.