Herein, we report the synthesis of zeolite composites with core shell structure via a secondary growth technique and evaluation of their catalytic performance in ethanol dehydration. In particular, SAPO-34 particles were functionalized by TPA(+), followed by dispersion in ZMS-5 or silicalite-1 to form SAP0-34@ZSM-5 and SAPO-34@silicalite-1 core shell materials showed a hierarchical porous structure consisting of both micropores and mesopores. The active sites in the developed composites were found to have a mild acidity. Compared to conventional zeolite catalysts in ethanol dehydration reaction, the silicalite-1 composites. The novel core shell materials showed a hierarchical porous structure consisting of both micropores and mesopores. The active sites in the developed composites were found to have a mild acidity. Compared to conventional zeolite catalysts in ethanol dehydration reaction, the core shell SAPO-34@ZSM-5 improved the selectivity toward light olefins. In addition, our catalyst test results revealed the enhancement in propylene and ethylene yield over SAP0-34@ZSM-5 and SAPO-34@siliclite-1, respectively, as compared to that of bare SAPO-34. An improved catalyst stability was also obtained for the composite materials owing to their core shell structure. The improved catalytic performance reported in this study reveals the potential utility of the zeolite composites with core shell structure in ethanol dehydration reaction.