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Abstract: A series of continuous, crack-free, highly ordered amino-functionalized mesoporous silica thin films have been directly synthesized by co-condensation of tetraethoxysilane (TEOS) and 3-aminopropyltriethoxysilane (APTES) in the presence of cationic CH3(CH2)15N+(CH3)3Br− (CTAB), nonionic C16H33(OCH2CH2)10OH (Brij-56) or triblock copolymer H(OCH2CH2)20(OCH(CH3)CH2)70(OCH2CH2)20)OH (P123) surfactant species under acidic conditions by sol–gel dip-coating. The molar ration of APTES/(TEOS+APTES) in the starting sol attains a value of 0.4. The effect of the sol aging on the mesostructure of thin films is systematically studied, and the optimal sol aging time is obtained for different surfactant systems. The amino-functionalized mesoporous silica thin films exhibit long-range ordering of 2D hexagonal (p6mm) and 3D cubic (Fm3m) pore arrays of size range from 2.2 to 8.3nm following surfactants extraction as demonstrated by XRD, TEM and physical adsorption techniques. Based on BET surface area and weight loss, the surface coverage of amino-groups for thin films prepared using different surfactants is calculated to be 3.2 and above amino-groups per nm2, which is very useful and promising for incorporating inorganic ions and biomolecules into these mesoporous silica materials. [Copyright &y& Elsevier]