Solar desalination of seawater is an effective approach to address the scarcity of freshwater resources. For solar steam generation, it is critical to design biodegradable, sustainable, low-cost, and high-evaporation-rate technology. This study aims to develop a novel solar desalination technology by designing and fabricating a nanocomposite material with excellent light absorption and thermal conversion properties. We designed a double-layer aerogel structure, which uses naturally abundant carboxymethyl cellulose (CMC) as the basic skeleton to achieve sustainability and biodegradability, and uses carbon nanotubes as the photothermal material for efficient light absorption to prepare a ferric tannate/carbon nanotube/carboxymethyl cellulose composite aerogel (FT-CNT-CMC aerogel). Experimental results demonstrate that the FT-CNT-CMC aerogel exhibits a high light absorption rate of 96–98% within the spectral range of 250–2400 nm, showcasing remarkable photothermal conversion performance. Under a sun intensity of 1 kW·m−2, the FT-CNT-CMC aerogel achieves a significant evaporation rate of 1.942 kg·m−2·h−1 at room temperature. Moreover, the excellent performance of the FT-CNT-CMC aerogel is validated in practical seawater desalination and organic dye wastewater purification. The FT-CNT-CMC aerogel exhibits a retention rate exceeding 99% for Na+, Mg2+, K+, and Ca2+ ions in simulated seawater, while no characteristic absorption peaks are observed in methylene blue and rhodamine B dye solutions after purification. These findings highlight the promising potential of the FT-CNT-CMC aerogel in the field of novel solar desalination, providing a viable solution to obtain freshwater.