Water scarcity has caused severe impact on the entire ecosphere while the climate change is resulting in high frequency of extreme weather conditions, especially extended period of drought. Due to the even increasing world’s population and the continued societal modernization, water scarcity is now one of the leading global challenges towards the development of human society. On the other hand, atmospheric water, accounting for 6 times the water in all rivers on Earth, is emerging as an alternative water resource. This dissertation thoroughly investigated the fully solar energy driven atmospheric water harvesting (AWH) process in a broad scientific and application context. The light-to-heat conversion process of solar photothermal materials was investigated first with a rationally designed droplet-laser system, which in combination with the calculation of heat of absorption of water vapor for various application scenarios, formed a theoretical basis of this dissertation research. As a result, a series of commonly used hydrated salts and their anhydrous counterparts were judiciously selected and successfully proven to be low-cost AWH materials to generate clean fresh water for arid regions. A hydrogel-deliquescent salt composite was further developed as AWH material with a significantly enhanced fresh water production capacity. A new design of nano-capsule encapsulated deliquescent salt was further put forward to enhance water vapor sorption/desorption kinetics, which enabled, for the first time, multiple sorption/desorption cycles within one day and thus multiplied water production capacity. The first-ever continuous AWH device, as opposed to batch-type one, was rationally designed, fabricated, and successfully tested in field conditions outdoors. At last, the dissertation pioneered a novel concept of atmospheric water sorption and desorption cycle for photovoltaic (PV) panel cooling. This dissertation shines significant light on sorption based atmospheric water harvesting and inspires more research efforts on this important research topic.