Atmospheric water is a resource equivalent to ~10% of all fresh water in lakes on Earth. However, an efficient process for capturing and delivering water from air, especially at low humidity levels (down to 20%), has not been developed. We report the design and demonstration of a device based on porous metal-organic framework-801 [Zr6O4(OH)4(fumarate)6] that captures water from the atmosphere at ambient conditions using low-grade heat from natural sunlight below one sun (1 kW per square meter). This device is capable of harvesting 2.8 liters of water per kilogram of MOF daily at relative humidity levels as low as 20%, and requires no additional input of energy.