Using zeolite MCM-22 as source and cetyltrimethylammonium bromide (CTAB) as template, mesoporous material denoted as M-MCM-22 with enhanced acidity has been synthesized and characterized by XPD, FT-IR, N-2 adsorption-desorption, 27Al-MAS NMR, IR spectra of pyridine adsorption, and NH3-TPD techniques, etc. The catalytic performance of M-MCM-22 was tested in alkylation of phenol with tert-butanol, indicating that M-MCM-22 showed highly and steadily catalytic properties. The highest conversion of phenol could be achieved at 418 K, while the highest selectivity to 2, 4-di-TBP was obtained at 398 K. It is found that high temperature is advantageous to form 4-TBP, whereas low weight hourly space velocity (WHSV/h-1) is helpful for both conversion of phenol and selectivity to 2,4-DTBP. It is also shown that high ratio of tert-butanol/phenol is beneficial for obtaining high conversion of phenol and selectivity to 2,4-di-TBP.