Zeolites are typically a class of crystalline microporous aluminosilicates that are constructed by SiO₄ and AlO₄ tetrahedra. Because of their unique porous structures, strong Brönsted acidity, molecular-level shape selectivity, exchangeable cations, and high thermal/hydrothermal stability, zeolites are widely used as catalysts, adsorbents, and ion-exchangers in industry. The activity, selectivity, and stability/durability of zeolites in applications are closely related to their Si/Al ratios and Al distributions in the framework. In this review, we discussed the basic principles and the state-of-the-art methodologies for regulating the Si/Al ratios and Al distributions of zeolites, including seed-assisted recipe modification, interzeolite transformation, fluoride media, and usage of organic structure-directing agents (OSDAs), etc. The conventional and newly developed characterization methods for determining the Si/Al ratios and Al distributions were summarized, which include X-ray fluorescence spectroscopy (XRF), solid state ²⁹Si/²⁷Al magic-angle-spinning nuclear magnetic resonance spectroscopy (²⁹Si/²⁷Al MAS NMR), Fourier-transform infrared spectroscopy (FT-IR), etc. The impact of Si/Al ratios and Al distributions on the catalysis, adsorption/separation, and ion-exchange performance of zeolites were subsequently demonstrated. Finally, we presented a perspective on the precise control of the Si/Al ratios and Al distributions of zeolites and the corresponding challenges.