Water harvesting from air in passive, adsorption‐based devices holds great potential for delivering drinking water to arid regions of the world. This technology requires adsorbents that can be tailored for a maximum working capacity, temperature response, and the relative pressure range in which reversible adsorption occurs. In this respect, metal–organic frameworks (MOFs) are promising, owing to their structural diversity and the precision of their functionalization for adjusting both pore size and hydrophilicity, thereby facilitating the rational design of their water‐sorption...