Cracking of tetralin and decalin was carried out over several zeolites to establish the effect of the pore topology of the catalyst on product distribution. These molecules were chosen as probe molecules, because they indicate which catalyst is the best for cracking or hydrotreating the light cycle oil (LCO) fraction, which is obtained directly from fluid catalytic cracking units. A set of zeolites with medium-sized (ZSM-5, MCM-22, ITQ-2), large (USY, Beta), and ultralarge pores (UTD-1), as well as a mesoporous MCM-41, were used as catalysts at 723 K. The results demonstrate that pore size and topology have a strong influence on diffusion, and consequently, on activity and selectivity in reactions such as ring opening, dealkylation, transalkylation, hydride transfer, and coke formation. UTD-1 generally has the highest activity per framework Al owing to the pore size and topology of this zeolite that enables flat molecules to diffuse easily inside the pores. According to the results, zeolites with medium-sized pores are adequate in combination with large-pore zeolites to crack naphthenes and fused aromatic-naphthenic rings, of the type present in LCO, to produce propene. Large-pore zeolites show good selectivity for naphthenic ring opening and appear to be better suited for hydrotreating LCO. Beta zeolite is a catalyst that is especially suitable for both processes.