The catalytic performance of zeolites is intrinsically linked to their structural and chemical properties. This review comprehensively explores how various structural and surface modifications enhance catalytic efficiency and fine-tune zeolite physicochemical properties. A key approach involves controlling the Si/Al ratio, which profoundly influences acidity and hydrothermal stability. Both bottom-up (synthesis) and top-down (post-synthesis) methods offer pathways to engineer specific acid site densities and introduce beneficial mesoporosity. Beyond composition, advancements in morphological control (2D nanosheets to 3D hollow particles) further enhance catalytic efficiency by effectively addressing diffusion limitations and extending catalyst lifetime. In terms of modulating the acid sites, the review highlights versatile approaches to metal incorporation, including isomorphous substitution for tuning framework acidity and various functionalization techniques–i.e., ion exchange, impregnation, and encapsulation–for creating spatially confined and highly dispersed metal nanoparticles on zeolite surfaces or within their internal sites. Case studies highlight the benefits of modifications in various catalytic reactions, including CO oxidation, methanol-to-olefins, and hydrodeoxygenation, demonstrating improved acidity, selectivity, and stability. The review concludes by outlining ongoing challenges related to optimizing synthesis methods to enhance one property without sacrificing others, advocating for integrated research combining advanced characterization with catalytic testing to establish robust structure-performance relationships of zeolite catalysts. © 2025 Wiley-VCH GmbH.