Ionothermal Synthesis of Metal‐Organic Frameworks Using Low‐Melting Metal Salt Precursors**

Abstract Metal‐organic frameworks (MOFs) are porous, crystalline materials constructed from organic linkers and inorganic nodes with myriad potential applications in chemical separations, catalysis, and drug delivery. A major barrier to the application of MOFs is their poor scalability, as most frameworks are prepared under highly dilute solvothermal conditions using toxic organic solvents. Herein, we demonstrate that combining a range of linkers with low‐melting metal halide (hydrate) salts leads directly to high‐quality MOFs without added solvent. Frameworks prepared under these ionothermal conditions possess porosities comparable to those prepared under traditional solvothermal conditions. In addition, we report the ionothermal syntheses of two frameworks that cannot be prepared directly under solvothermal conditions. Overall, the user‐friendly method reported herein should be broadly applicable to the discovery and synthesis of stable metal‐organic materials.