A thin TS-1 zeolite film was successfully fabricated on palladium membrane using an assembly method combined with secondary growth technique. The preparation of TS-1-Pd composite membrane involved three stages: (1) deposition of palladium layer on porous alumina support through electroless plating; (2) assembly of silicalite-1 zeolite seeds on the palladium layer; (3) growth of TS-1 layer from the zeolite seeds over the top surface of the palladium layer using hydrothermal synthesis method. The detailed microstructure of the TS-1-Pd composite membrane was examined by SEM, EDX, XRD, FT-IR and UV vis. This architecture allows the composite membrane to remain stable for 10 days of hydrogen permeation tests at 773 K and tolerate 30 cycles in gas exchanging tests, even for 5 days of hydrogen permeation tests at 423 K. Furthermore, the presence of a TS-1 zeolite film on palladium membrane effectively protected the palladium membrane from the contamination from the hydrocarbon, therefore greatly enhanced its operation stability. (C) 2017 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.