Heteroatoms of Al and Ti are effectively introduced into the framework of ordered mesoporous silica materials (designated as MAS-7 and MTS-9, respectively) in strong acidic media (pH < 0) by a two-step procedure. MAS-7 shows high catalytic activities for the cracking of both small (cumene) and bulky (1,3,5-triisopropylbenzene) molecules because it combines the advantages of both zeolites (strong acidity) and mesoporous materials (large pores). In contrast, Al-SBA-15 samples prepared from both "post-synthesis" and "direct synthesis" present much lower catalytic activities than MAS-7. Furthermore, MTS-9 exhibits very high catalytic activity in phenol hydroxylation by H2O2, giving the phenol conversion of 26%, comparable to TS-1.