Due to the ever-growing global population, it is necessary to develop highly effective processes that minimize the impact of human activities and consumption on the environment. The levels of organic and inorganic contaminants have rapidly increased in recent years, posing a threat to ecosystems. Removing these toxic pollutants from the environment is a challenging task that requires physical, chemical, and biological methods. An effective solution involves the use of novel engineered materials, such as silica-based nanostructured materials, which exhibit a high removal capacity for various pollutants. The starting materials are also thermally and mechanically stable, allowing for easy design and development at the nanoscale through versatile functionalization procedures, enabling their effective use in pollutant capture. However, improvements concerning mechanical properties or applicability for repeated cycles may be required to refine their structural features. This review focuses on hybrid/composite polymer-silica nanostructured materials. The state of the art in nanomaterial synthesis, different techniques of functionalization, and polymer grafting are described. Furthermore, it explores the application of polymer-modified nanostructured materials for the capture of heavy metals, dyes, hydrocarbons and petroleum derivatives, drugs, and other organic compounds. The paper concludes by offering recommendations for future research aimed at advancing the application of polymer-silica nanostructured materials in the efficiency of pollutant uptake.