Abstract: Toluene was alkylated with methanol to produce xyienes rich in the para iso-mcr over ZSM-5 zeolites modified with alkali compounds by ion-exchang, impregnation, and mechanical mixing. At reaction conditions, the conversion of toluene and para isomer in the xylene product were 33.9% and 79.4% respectively using the zeolite catalyst which was modified by sodium cation exchang followed by rapid impregnation with sodium acetate. The selectivity of p-xylene was also enhanced by poisoning the catalysts with nitrogenous bases. It was observed that the higher the p-xylene selectivity in toluene alkylation with methanol, the lower the catalytic activity in xylene isomerization over the same catalysts. The results of studies on surface properties by TPD, pyridine pulse poisoning, and BETweight methods indicated that the total acidity was decreased, the acid strength was weakened, and the relative sorption capacity of p-xylene vs. m-xylene was enhanced after modifying with alkali compounds.