The objective of this work is to give a comparative characterization of the three-dimensional (3D) MSU-2 and unidimensional (1D) MCM-41-like aluminosilicates, in particular with respect to acidity and catalytic properties in 1,3,5-triisopropylbenzene cracking. Mesoporous AIMSU-2 with wormhole but uniform pores and large surface area, previously obtainable only from silicon alkoxides, has been successfully prepared from pre-assembled zeolite-like units in the presence of nonionic octyl-phenyl polyethylene ether (TX-100) as template through a N-0(N+)X-I+ pathway in strong acid media. For comparison purpose, hexagonally ordered AIMCM-41 was also synthesized from the same inorganic precursor with cetyltrimethylammonium bromide (CTAB) as template under mild basic conditions. Catalytic results in bulky 1,3,5-triisopropylbenzene cracking showed that the 3D AIMSU-2 was much more active than the hexagonally packed AIMCM-41 though both materials were synthesized from the same precursor and presented similar acid strength. (C) 2004 Elsevier B.V. All rights reserved.