Tremendous efforts have been made in recent years to synthesize ordered mesoporous zeolite materials, because of the accelerating demands of industrial bulky molecule conversion. Here, we develop a novel gradient acidic assembly growth strategy to prepare ordered highly zeolitized mesoporous aluminosilicate (SBA-16) materials in a mixed template system. This gradient acidic assembly growth strategy can achieve the high zeolitization of mesoporous aluminosilicate walls without any ordering loss of the mesostructure. The resultant highly zeolitized mesoporous materials, composed of the intergrown zeolite subcrystal particles (2-3 nm), exhibit high surface area (∼834 m2 g-1) and pore volume (∼0.64 cm3 g-1), typical channel of MFI framework (0.52 nm), and uniform mesopore (∼5.75 nm), respectively. Moreover, these highly ordered crystallized mesostructures endow them with high exposed active sites and excellent hydrothermal stability, which consequently make their catalytic activities in bulky molecule transformations at least 10 times higher than conventional zeolites or amorphous mesoporous materials. Without the use of any special surfactants, this general synthetic process provides a brand new view for the synthesis and application of highly crystalline ordered mesoporous materials.