Novel hybrid mesoporous and functionalized materials with controllable surface area and pore dimensions with functional basic sites (-NH2) were synthesized from magadiite and [Al]-magadiite as layered silicate precursors. The variable pore structure and properties of these materials were investigated in these solids by using different CTA(+)/Na(+) (CTA(+) = cetyltrimethylammonium cation) molar ratios in the pre-modification step with aminopropyltriethoxysilane (APTS) and tetraethoxysilane (TEOS). Characterizations were carried out by different techniques to probe the effects of the amounts of interlayer surfactant in the synthesis of the pillared and/or grafted materials. The crystalline structures of magadiite and [Al]-magadiite layers were maintained as evidenced by FT-IR and SAED and contain pillars and aminopropyl groups in the interlayer space. The hybrid solids were compared to the pillared forms (H. M. Moura, F. A. Bonk and H. O. Pastore, Eur. J. Mineral., 2012, 24, 903) and to the aminopropyl-grafted forms and presented the properties of both solids with the CO2 adsorption capability improved considerably.