Atmospheric water is an abundant alternative water resource, equivalent to 6 times the water in all rivers on Earth. This work screens 14 common anhydrous and hydrated salt couples in terms of their physical and chemical stability, water vapor harvesting, and release capacity under relevant application scenarios. Among the salts screened, copper chloride (CuCl2), copper sulfate (CuSO4), and magnesium sulfate (MgSO4) distinguish themselves and are further made into bilayer water collection devices, with the top layer being the photothermal layer, while the bottom layer acts as a salt-loaded fibrous membrane. The water collection devices are capable of capturing water vapor out of the air with low relative humidity (down to 15%) and releasing water under regular and even weakened sunlight (i.e., 0.7 kW/m2). The work shines light on the potential use of anhydrous salt toward producing drinking water in water scarce regions.