A comprehensive study has been made on the cracking abilities of mesoporous aluminosillicate MCM-41 materials with different Si/Al ratios (15-?) and pore diameters (1.6-3.0 nm) by using 1,3,5-triisopropylbenzene (1,3,5-TiPB) cracking as the test reaction. The roles of Al content and pore diameter on the catalytic features of the samples were evaluated by the conversion of 1,3,5-TiPB, coke content and deactivation parameters. It is found that the catalytic activity is mainly controlled by adsorptive properties towards the reactant and the dispersion of acid sites. In terms of their catalytic performances, cracking reaction over aluminosilicate mesoporous materials is more favorable for catalysts with smaller pore size and higher Al concentration. Moreover, coking is found responsible for catalyst deactivation during 1,3,5-TiPB cracking reaction over Al-MCM-41.