Abstract: The ongoing expansion of human activities and unsustainable production practices have led to the extensive release of pollutants into the environment, posing a substantial threat to both ecological systems and human health. To facilitate continuous environmental monitoring and enable timely pollution control, there is an urgent demand for the development of ultrasensitive detection technologies for trace pollutants. Over recent decades, fluorescence, electrochemical, and surface-enhanced Raman scattering techniques have been widely utilized for detecting pollutants such as explosives, pesticides, heavy metal ions, and antibiotics. Among these methods, detection sensitivity is highly dependent on the sensing material, underscoring the critical importance of material development in advancing these technologies. In comparison to low-dimensional sensing materials, three-dimensional aerogels exhibit advantageous properties such as high specific surface area, low density, and high porosity. Additionally, their tunable constituent units have attracted considerable attention in the field of trace pollutant detection. This paper reviews detection technologies based on aerogel materials, highlighting several typical aerogel materials and discussing their applications in detecting various types of environmental pollutants. Finally, considering the current state of research, the challenges and future prospects for the development of aerogel materials are discussed.