It is shown that the alkylation of toluene with ethylene to give p-ethyltoluene can be conducted selectively on small crystals (less-than-or-equal-to 1-mu-m) of unmodified H-ZSM-5 zeolites to a level higher than that corresponding to a thermodynamic equilibrium composition. A comparison of the ethyltoluene isomers formed with H-Y and H-ZSM-5 zeolites at various conversions and temperatures indicates that p-ethyltoluene is preferentially formed in the channel intersections of the H-ZSM-5 zeolite, even during the initial alkylation step. The final ethyltoluene isomer composition is a result of competition between the rates of alkylation and isomerization and subsequent diffusional transport of individual isomers through the zeolite channels. Zeolite coking causes an apparent increase in the p-ethyltoluene selectivity; however, a more dramatic decrease in toluene conversion results in the formation of a considerably lower amount of p-ethyltoluene. This is caused by a partial blocking of the zeolite channel system.