This review explores the multifaceted role of functionalized mesoporous silica in removing both inorganic and organic pollutants from various environmental matrices. The growing interest in mesoporous silica for pollution remediation was examined. The synthesis and analysis of organosilica materials with mesoporous structures were discussed, highlighting their unique properties and potential applications. The review explains the mechanisms behind the adsorption of inorganic contaminants like heavy metals. It highlights the interaction of mercury (Hg(II)) with thiol-functionalized mesoporous silica and the effectiveness of amino, poly-amino groups, advanced ligands, and bi-functionalized adsorbents. It also discusses the selectivity and functionality of these materials, focusing on their ability to target specific pollutants and reduce environmental harm. Furthermore, the review addresses the crucial aspect of regeneration and reuse of absorbent materials, enhancing the sustainability of pollution remediation processes. In addition to inorganic pollutants, the review examines the adsorption of hazardous organic species by pristine and uncalcined mesoporous silica, as well as aluminum-containing mesoporous silica. The incorporation of cyclodextrins into mesoporous silica matrices is explored as a strategy to enhance the adsorption capacity of organic compounds. Oxyanions and radionuclides are also considered, underscoring the versatility of mesoporous silica-based adsorbents in addressing a wide range of environmental contaminants. This review provides insights into the potential of enhanced mesoporous silica as a versatile and efficient solution for the removal of both inorganic and organic pollutants, paving the way for sustainable environmental remediation strategies.