Mesoporous aluminosilicate molecular sieves, Al-contaming MCM-41, with different Si/Al ratios were synthesized by four different methods: sol-gel, hydrothermal, template cation exchange and grafting. The catalysts prepared by sol-gel, grafting and template cation exchange methods are effective for the incorporation of large amounts of aluminum into the framework of MCM-41. The catalytic activities of the resulting Al-containing MCM-41 samples were tested in the cracking of cumene and the dehydration of 2-propanol, as model acid-catalyzed reactions, and then compared with the results obtained from microporous H-ZSM-5 and HY zeolites. The Al-containing MCM-41 catalysts prepared by different methods behaved differently in acting as acidic catalysts; the catalyst (having almost same Si/Al ratio) prepared by sol-gel method showed higher cracking activity, whereas that prepared by template cation exchange method showed higher dehydration activity. Moreover, these Al-containing MCM-41 catalysts are more catalytically active than microporous HY zeolite for cumene cracking and 2-propanol dehydration reactions. (C) 2002 Elsevier Science B.V. All rights reserved.