A zeolite capsule catalyst Cr/ZnO-S-Z was prepared successfully by a novel dual-layer method, in which one layer of neutral Silicalite-1 zeolite shell was first synthesized on the bimetallic Cr/ZnO core catalyst, acting as the intermediate layer for the following H-type H-ZSM-5 zeolite shell direct synthesis on its surface. By using this dual-layer method, it can be easily realized that the formation of H-ZSM-5 zeolite membrane on the millimeter-sized bimetallic substrates. Direct synthesis of dimethyl ether (DME) from syngas at higher reaction temperature was the application of this zeolite capsule catalyst to test its catalytic performance. In reaction, this zeolite capsule catalyst could realize the exactly controlled synthesis of DME, suppressing the formation of other alkane/alkene by-products simultaneously, demonstrating its exclusive ability for the selective synthesis of target product compared with the conventional hybrid catalyst. (C) 2011 Elsevier B.V. All rights reserved.