Water and energy scarcity are the challenges for humankind in the coming years. Sun is the largest source of energy available on the planet. Also, brackish seawater covers more than 70% of the surface of the planet. Therefore, combining these two valuable natural resources represents an appealing solution to overcome the problem of sweet water shortage. To achieve this goal, the missing link is to develop appropriate photothermal materials with efficient light-to-heat-to-vapor generation. In this work, green moss is introduced as a natural, eco-friendly, abundant, superhydrophilic, fast water transporter, salt rejector, and highly efficient solar collector material. Green moss, owing to its open-microgrooves, can supply adequate water to the evaporation surface, while its open capillary channels can reject the precipitated salt, allowing its reusability. The green moss solar steam generator demonstrated an outstanding solar evaporation rate of 2.61 kg m–2 h–1 under 1 sun illumination, which is much higher than other reported natural and chemically modified biomasses under otherwise similar conditions. Interestingly, upon chemical modification of the green moss surface, it is possible to increase its solar evaporation rate to >3 kg m–2 h–1. Using the moss to purify and desalinate brackish water, it was demonstrated that it has the ability to decrease salinity below the WHO standards for drinkable water.