Shape-selective zeolites (HZ-x/y) were synthesized by a one-pot method using TPAOH (y) and/or MeEt3N+I (x) as templates. The use of MeEt3N+I affects the crystal growth and the distribution of acid sites on the external surface of the zeolites. The catalysts show excellent catalytic activity towards toluene alkylation with CH3Br. With toluene conversion of 36.3% and p-xylene selectivity of 66.2%, HZ-40/0 is the most effective among the prepared catalysts, showing a p-xylene yield of 21.2%. The improved para-selectivity is mainly due to the decrease of acid sites on the external surface of the catalysts. (C) 2018 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co., Ltd. All rights reserved.