Mesostructured aluminum phosphonates (AOP-x) bridging with 1,1'-hydroxyl ethylidene groups, including a lamellar mesostructure (AOP-N) with crystalline framework, a well-ordered 2D-hexagonal mesophase (AOP-Cl), and a particle-packed mesostructure (AOP-S), were simply synthesized in the presence of surfactant cetyltrimethylammonium bromide in the ethanol-water system, by choosing Al(NO3)(3), AlCl3 and Al-2(SO4)(3) as the aluminum source, respectively. The crystallinity, morphology, mesophase, and skeletal structure of the as-prepared materials were characterized by XRD, TEM, SEM, (27)AI, P-31 and C-13 MAS NMR, and nitrogen sorption techniques. After calcination under N-2 at 350 degrees C, the calcined AOP-x samples consist of aluminum phosphonate and phosphate, possessing desirable specific surface areas of 116-585 m(2)/g. The effect of the inorganic counteranions (NO3-, Cl- and SO42-) from the aluminum source on the formation of different AOP-x mesostructures was discussed in terms of their bind strength to the headgroups of the surfactant micelles, suggesting the potential for designed synthesis of non silica -based mesostructured organic-inorganic hybrid materials. (C) 2018 Elsevier Inc. All rights reserved.