In order to improve the separation performance of pervaporation (PV) membranes, different silicalite-1 particles were prepared by hydrothermal synthesis in fluoride (F) or alkaline (OH) media, and then incorporated into polydimethysiloxane (PDMS) to prepare PDMS/silicalite-1 PV membranes. These silicalite-1 particles were characterized by SEM, FT-IR, NMR, XRD, BET and IGA. The results indicated that, compared with the silicalite-1(OH), the silicalite-1(F) particles had much less silanol groups and were more hydrophobic, thus showing higher selectivity to ethanol. Accordingly, the separation factor (ethanol/water) of the PDMS/silicalite-1(F) membrane was much higher than that of PDMS/silicalite-1 (OH) membrane at the same silicalite-1 loading. For the PDMS/silicalite-1(OH) membrane, the highest separation factor (23.0) was obtained at 60 wt% silicalite-1 loading, while it was found to be 23.8 at 40 wt% silicalite-1 loading for the PDMS/silicalite-1(F) membrane. However, due to the larger size of the silicalite-1(F) particles, its maximal loading (40 wt%) in PDMS was lower than that of the silicalite-1(OH) particles (60 wt.%). In order to Lake advantage of the higher selectivity of silicalite-1(F) particles and the higher loading of silicalite-1(OH), these two kinds of silicalite-1 particles were mixed and incorporated into PDMS. Using this new strategy, the total loading of the silicalite-1 particles could be up to 60 wt%, and the separation factor of such membrane increased to 28.9 when he partial loading of silicalite-1 (F) was 30 wt%. The effects of feed temperature and ethanol concentration on this new PDMS/silicalite-1 (F)-silicalite-1(OH) membrane were also investigated. The results demonstrated that the incorporation of the mixed silicalite-1(F) and silicalite-1(OH) particles into PDMS could be a promising method for the preparation of high performance PV membranes. (C) 2015 Elsevier B.V. All rights reserved.