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This data set systematically investigates the structural regulation, acidity evolution, catalytic performance, and coke formation behavior of HZSM-5 zeolites modified synergistically with levulinic acid (LA) and Zn (L/Zn0.2-ZSM5). It comprises characterization and catalytic evaluation data obtained from XRD, N₂ adsorption–desorption, NH₃-TPD, Py-FTIR, XPS, FTIR, Raman, and TGA analyses, totaling 12 data files.Specifically, Files 1–4 contain XRD, N₂ adsorption–desorption, NH₃-TPD/Py-FTIR, and XPS data of fresh HZSM-5 zeolites before and after modification, which are used to elucidate the effects of synergistic modification on crystal structure, pore structure, acidity characteristics, and the chemical states of Zn species. Files 5–6 provide the raw catalytic data, including methanol conversion, oil-phase yield, BTX selectivity, and product distribution, for different HZSM-5 catalysts and L/Zny-ZSM5 (y = 0.1, 0.2, 0.6, and 2.0 wt%) with varying Zn loadings in the methanol-to-aromatics (MTA) reaction. Files 7–11 present XRD, FTIR, Raman, TGA, and N₂ adsorption–desorption data of the spent HZSM-5 zeolites, enabling analysis of structural stability, coke chemical composition, degree of graphitization, and coke-induced pore structure evolution during reaction. File 12 contains the graphical abstract of this work.Overall, this data set systematically elucidates the synergistic interplay among pore architecture, acidity modulation, and active site evolution in HZSM-5 zeolites during the MTA reaction, providing reliable data support for the rational design and performance optimization of high-performance MTA catalysts.