The development of recyclable solid acids is of major industrial importance and challenging in many reactions, for instance, the Friedel-Crafts alkylation as one of the most prevalent examples, which generally requires the presence of acid catalysts. However, not only the replacement of traditional toxic acid catalyst by solid acidic zeolites but also the improvement such catalysts in term of high efficiency has been addressed through environmental technologies. Our present study explores the use of hierarchical faujasite zeolite nanosheets as catalysts in industrial applications with the frame of development of green and sustainable technologies. The simple and efficient route to prepare the faujasite zeolite with the nanosheet-assembled structure together with the roles of synthetic parameters on the characteristics and properties are systematically investigated. This first example of hierarchical zeolite, which has uniform mesoporous features derived from the interstitial pores between the nanosheet assemblies, exhibits a superior catalytic activity in terms of conversion and selectivity for the benzylation of toluene with benzyl chloride. In conclusion, the fine-tuning of structural characteristics of zeolites by a simple optimization of surfactant contents and crystallization temperatures allows the design of the candidate catalyst for a green and sustainable future. This work also demonstrates the next step forward in the development of an industrial catalyst based on the concept of cleaner production.