Organically modified silicate (ORMOSIL) materials have emerged as highly efficient catalysts in advanced organic synthesis due to their hybrid nature, which combines the structural stability of silica with tunable organic functionalities. Their versatility has driven significant advancements in various catalytic applications. In heterogeneous catalysis, ORMOSIL-based catalysts offer high surface area, stability, and reusability, facilitating efficient interactions with reactants and improving reaction rates and selectivity. Moreover, in acid-base catalysis, functionalization with acidic (e.g., sulfonic acid) or basic (e.g., amine) groups enables transformations such as aldol condensation, esterification, and transesterification with enhanced efficiency and recyclability. Additionally, ORMOSIL plays a crucial role in asymmetric synthesis by serving as a robust support for chiral catalysts, improving enantioselectivity and stability in reactions such as asymmetric hydrogenation. Its porous structure makes it an excellent material for enzyme immobilization, preserving enzymatic activity and promoting sustainable biocatalytic transformations. Furthermore, ORMOSIL-based photocatalysts, often combined with metal or semiconductor nanoparticles, exhibit enhanced light absorption and charge separation, making them highly effective in oxidative and reductive photocatalytic reactions. In electrocatalysis, ORMOSIL enhances catalyst stability and conductivity, facilitating redox reactions in electrochemical organic synthesis, including applications in fuel cells. The integration of ORMOSIL with nanomaterials and other catalytic components has led to the development of multifunctional catalytic systems with superior performance, selectivity, and sustainability. This review provides an in-depth exploration of these advanced catalytic applications, highlighting recent progress and future prospects in ORMOSIL-based catalytic systems for organic synthesis.