Using high-performance catalysts prepared from zeolites Y, M, and ZSM-5, the dependence on the acid and micropore characteristics of modified zeolites was studied for the yields of products of dehydrocycloaromatization of C2+ alkanes, the isomerization of n-pentane, and the disproportionation of toluene. On the basis of the obtained experimental results and published data, it was shown that the initial activation of reactant molecules occurs on acid sites regardless of their acid strength and that the formation and rearrangement of C-C bonds are controlled by the molecular-sieve parameters of a zeolite and can be varied via the modification of the virgin zeolites used to prepare the catalysts.