Ordered mesoporous aluminosilicates have been successfully obtained via the simple combination of top-down and bottom-up approaches, using commercially available zeolites as the framework sources. The mesoporous aluminosilicates are characterized by XRD, N-2 sorption, SEM, TEM, ICP, and NMR, and have proven to have controllable aluminium contents, well-developed mesoporosity, and excellent hydrothermal stability. The hydrothermally stable mesoporous aluminosilicates, which possess the proper distribution of weak and strong acid sites, are applied as reusable heterogeneous catalysts for the pyrolysis of woody biomass. The mesoporous alummosilicates in the present work showed good activity, selectivity, and even stability for the production of desirable organic compounds such as phenolics, in comparison to conventional HZSM-5 and Al-MCM-41. (C) 2008 Elsevier B.V. All rights reserved.