Recycling polluted water via different techniques has become one of the most feasible ways to solve the freshwater crisis. We describe a novel method to prepare reusable and efficient photothermal energy conversion materials for water purification. Using crosslinked xerogels as precursor, the porous and interconnected carboxymethylcellulose sodium-derived carbon aerogels (abbreviated as CCAs) with good hydrophilic performance and strong light absorption capability are firstly fabricated through pyrolysis. Photothermal measurement results show that CCA15 exhibit excellent solar steam generation rate of 2.31 kg m−2 h−1 with high light-to-vapor conversion efficiency of 95.9% under 1 sun illumination. In addition, the feasible application of CCA15 for efficient water purification under 1 sun irradiation using a homemade water treatment device has been demonstrated successfully. The as-prepared CCAs shown in here can be a continuable solution to mitigate the global freshwater crisis.