Vapor-phase methylation of toluene with methanol and isopropylation of toluene with 2-propanol has been investigated in a down flow reactor under atmospheric conditions using N₂ gas carrier over a series of surface modified and unmodified ZSM-5 (Si/Al=60–170) loaded with H₃PO₄, differing in the external surface treatment of the zeolites. The feed molar ratios of toluene/methanol and toluene/2-propanol were varied over a wide range (8–0.125), and the optimum feed ratio of toluene/alcohol was less than 0.5 in both cases. Space velocity employed in toluene methylation reported as WHSV (toluene)=1.2h⁻¹, and the space velocity employed in toluene isopropylation reported as WHSV (toluene)=0.8h⁻¹. The methylation reactions were carried out in the temperature range of 623–773K, and the isopropylation reactions were carried out in the temperature range of 483–583K. Atmospheric pressures was maintained in all runs. Catalysts containing 0–4.9wt.% P were prepared using modified and unmodified ZSM-5 zeolites, and their catalytic performance for vapor-phase alkylation of toluene with methanol and 2-propanol were investigated. The optimum phosphorous content for methylation was 2.1wt.% P which was greater than the optimum phosphorous loading for isopropylation (0.7wt.% P).