When fabricating macroscopic devices exploiting the properties of organic chromophores, the corresponding molecules need to be condensed into a solid material. Since optical absorption properties are often strongly affected by interchromophore interactions, solids with a well‐defined structure carry substantial advantages over amorphous materials. Here, the metal–organic framework (MOF)‐based approach is presented. By appropriate functionalization, most organic chromophores can be converted to function as linkers, which can coordinate to metal or metal‐oxo centers so as to yield stable, crystalline frameworks. Photoexcitations in such chromophore‐based MOFs are surveyed, with a special emphasis on light‐switchable MOFs from photochromic molecules. The conventional powder form of MOFs obtained using solvothermal approaches carries certain disadvantages for optical applications, such as limited efficiency resulting from absorption and light scattering caused by the (micrometer‐sized) powder particles. How these problems can be avoided by using MOF thin films is demonstrated.

Design strategies and applications of metal–organic frameworks (MOFs) showing charge transfer properties are discussed.