The importance of water cannot be overstated. It is the most important natural resource for our survival and development. The development of suitable materials for efficient water purification will provide a critical contribution for sustainable water use. In this context, a gel–emulsion‐templated synthesis of a polymeric aerogel has been developed for water treatment. Owing to its hydrophobic nature, the aerogel shows high sorption (nearly 20 times its weight) for organic liquids, such as toluene, phenol, and nitrobenzene, and can be used to remove them from water. The aerogel shows low thermal conductivity (0.032 W m−1 K−1) and excellent light absorption efficiency (>92 %) after carbonization, which provides the possibility for the construction of an interfacial solar vapor generation system. The as‐prepared materials are used to develop a two‐step approach to remove both organic and inorganic contaminants (salts) from water. Importantly, the aerogel shows excellent reusability and high efficiency both for oil sorption and for solar vapor generation. Moreover, the low cost and easy scale‐up of the preparation process lay a solid foundation for practical application. It is anticipated that the prepared aerogels would contribute not only to water purification but also to other related areas.