The alkylation of 1, 2, 4-trimethylbenzene (1, 2, 4-TrMB) with methanol on HZSM-5 type zeolites with various aluminium concentrations was studied in a fixed bed type apparatus with a continuous flow system at atmospheric pressure. It was found that 1, 2, 4, 5-tetramethylbenzene (1, 2, 4, 5-TeMB), which was the smallest isomer in TeMB, could be produced at a very high selectivity by application of the shape selectivity of HZSM-5 zeolites. HY and H-mordenite, which had larger pore window size than HZSM-5, showed higher catalytic activity for this alkylation than HZSM-5. On HY and H-mordenite, however, the fraction of 1, 2, 4, 5-isomer in TeMB produced was lower than that on HZSM-5. With the increase of aluminium concentration in HZSM-5, the yield of TeMB increased, while the fraction of 1, 2, 4, 5-isomer in the produced TeMB decreased. From these results it is concluded that 1, 2, 4, 5-TeMB is mainly formed in the pores of HZSM-5 in which the rate of reaction may be controlled by the diffusion of reactants and products. The other isomers of TeMB, TrMB except 1, 2, 4-isomer and pentamethylbenzene are formed on the outer surface of HZSM-5 crystallites.