New and ordered 2D-hexagonal (p6mm) mesoporous aluminosilicates (CMI-11) have been synthesized in strongly alkaline media using aluminosilicate ester (((BUO)-O-s)(2)-Al-O-Si-(OEt)(3)) as single-source molecular precursor and CTMABr as surfactant and characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), N-2 adsorption-desorption and Al-27 and Si-29 MAS NMR spectroscopy. These mesoproous alummosilicates exhibit a very low SUM ratio of 1.9 and highly thermal stable tetrahedral aluminum sites in the mesoporous walls. Al-27 and Si-29 MAS NMR spectroscopy indicates that the pore walls of CMI-11 are fully condensed with molecular homogeneity of Si-O-Al linkage. These materials are highly important in catalysis, in particular for the petroleum processing and the bulky molecules treatment. (c) 2007 Elsevier B.V. All rights reserved.