Hierarchical zeolites can provide multidimensional spatial networks and, therefore, have significant potential as catalysts for the cracking of biomass to generate light olefins. The present work synthesized the diquaternary ammonium-type surfactant [C 18 H 37 −N + (CH 3 ) 2 −(CH 2 ) 6 −N + (CH 3 ) 2 −C 6 H 13 ]Br 2 , incorporating hydrophobic 18-carbon alkyl groups for usage as a structure-directing agent. This compound was subsequently used to prepare nanosheets of a hierarchical ZSM-5 two-dimensional zeolite (HNZSM-5) through a one-pot hydrothermal method. The crystal phase, morphology, and hierarchical structure of the HNZSM-5 were analyzed using various techniques, including X-ray diffraction, electron microscopy, and N 2 adsorption/desorption. When applied to the catalytic cracking of a waste cooking oil model compound, the HNZSM-5 exhibited superior activity and stability compared with a conventional ZSM-5. This performance was attributed to the more accessible acid sites and unique lamellar structure of the former material. The HNZSM-5 also outlasted the conventional zeolite, showing deactivation after 45 h of reaction compared with 20 h, indicating exceptional stability and excellent resistance to coking.