Metal-organic frameworks (MOFs) have been extensively studied over the last two decades due to their high degree of synthetic tunability, which makes it possible to tailor their physical and chemical properties for a given application. While much attention has been focused on the use of MOFs for industrial gas storage and separations, the design of MOFs with targeted electronic properties has become a topic of recent interest as well. Through a judicious selection of inorganic nodes and organic linkers, MOFs have been proposed for novel (opto)electronic devices, electrocatalysts, photocatalysts, sensors, and energy storage devices, among many other applications. However, with tens of thousands of MOFs that have been experimentally synthesized and virtually unlimited more that can be proposed, it is often difficult to identify promising MOF candidates with the optimal set of electronic properties.