A novel zeolite-modified alumina-bead catalyst (ZSM-5/Al2O3-b) was prepared via calcining zeolite-coated alumina-bead material (Al2O3-b@ZSM-5) to graft zeolitic acid sites on the alumina-bead surface. The acid catalyst proved high activity and more 8 times catalytic efficiency than the corresponding ZSM-5(5 %) + Al2O3 mechanically mixed catalyst for cracking of 1, 3, 5-triisopropylbenzene (TIPB) in the FCC simulation reactor with short contact time. The characterization results showed that the surface property of the alumina-beads has been modified and the interface connection of Si-O-Al bonds between zeolitic nanoparticles and alumina resulted in stable zeolite particles on the alumina surface and the structural stability in hot water. The excellent catalytic performances are ascribed to the decrease of diffusion limitation of reactants and intermediates and the increase of Brønsted acid sites on the ZSM-5/Al2O3-b catalyst. The grafted/modified alumina-bead catalyst can be directly used in practical catalytic cracking of large molecules without forming. This strategy can be extended to the preparation of other types of zeolite-containing catalysts and industrial applications.