t-Butylation of 4-methoxyphenol (4-MP) with t-butylalcohol (t-BuOH) as alkylating agent have been conducted under liquid phase reaction conditions over Zn-Al-MCM-41 catalysts with different n(Si)/(n(Zn) + n(Al)) ratios for selective synthesis of 2-t-butlylated hydroxyl anisole (2-TBHA). The influences of various reaction parameters such as reaction temperature, time and t-BuOH to 4-MP ratios on the conversion of 4-MP and the selectivity of 2-TBHA have also been studied. With the decrease of the n(Si)/(n(Zn) + n(Al)) ratios of Zn-Al-MCM-41 catalysts from 380 to 75, the conversion of 4-MP as well as the yield and selectivity of 2-TBHA increase due to the increase of the number of Bronsted acid sites in Zn-Al-MCM-41 catalysts. The n(Si)/(n(Zn) + n(Al)) ratio of 75 is found to be the most suitable and reusable for the t-butylation of 4-MP with t-BuOH for selective synthesis of 2-TBHA. (c) 2006 Elsevier B.V. All rights reserved.