Significant improvements in both the hydrothermal stability and the acidity of mesostructured aluminosilcates have been reported recently. New assembly pathways, along with post-synthesis treatment methods, have made it possible to form structures with thick and more highly crosslinked framework walls. The resulting structures are slow to degrade under hydrothermal conditions in comparison to conventional analogs. Also, improved methodologies for grafting Al centers into the walls of pre-assembled frameworks have afforded aluminosilicate mesostructures with enhanced acidity. The most promising strategy for improving the hydrothermal stability and acidity of aluminosilicate mesostructures, however, is based on the use of protozeolitic nanoclusters. These so-called “zeolite seeds” can be directly assembled into hexagonal, cubic, wormhole, and foamlike framework structures under a variety of assembly conditions. They also can be grafted into the walls of pre-assembled frameworks to form more stable acidic derivatives.