The HSE06 functional is a screened-exchange functional built upon PBE and replaces a portion of PBE's local exchange with 25% HF exchange at small interelectronic distances, decreasing continuously to zero at large interelectronic distances. HSE06 was selected in this work because it is currently the most widely used functional for predicting the band gaps of solid-state materials when high accuracy is required, including for MOFs. Other functionals may have comparable or slightly better performance for certain systems but are less widely used and tested. In addition to HSE06, we considered the hybrid functional defined here as HSE06 * , which has 10% HF exchange at small interelectronic distances and decreases to zero at large interelectronic distances. HSE06 * was considered because the standard HSE06 functional can overcorrect the band gap underprediction problem of PBE for some materials, as is the case with MOF-5. Considering a functional with an intermediate fraction of HF exchange between that of PBE and HSE06 also makes it easier to discern the impact of HF exchange. The HSE06 and HSE06 * calculations are considerably more expensive than the PBE calculations because of the nonzero fraction of HF exchange. With this in mind, we included the HLE17 meta-GGA functional as well because prior benchmarking studies suggest that it can greatly improve the prediction of semiconductor band gaps without the need for computationally expensive HF exchange. While one could also consider the GGA+U approach, relatively little is currently known about selecting empirically ideal U values for MOFs despite its widespread use in correcting the predicted energetic and electronic properties of inorganic solids in high-throughput DFT databases. For materials that are closed-shell (i.e. without magnetic character), the band gap is defined as the energy difference between the conduction band minimum (CBM) and valence band maximum (VBM). For materials with open-shell character, there can be more than one way to characterize the band gap. Except where otherwise stated, we define the band gap for spin-polarized systems as min(CBM ↑ , CBM ↓ )max(VBM ↑ , VBM ↓ ), where ↑ and ↓ refer to the spin-up and spin-down spin-orbital manifolds, respectively. Nonetheless, we note that this definition can occasionally result in a band gap that is associated with a formally spin-forbidden electronic excitation, as depicted in Figure . Using the band gap instead defined as min(CBM ↑ -VBM ↑ , CBM ↓ -VBM ↓ ) does not involve a spin-flip. Regardless of which band gap definition is employed, the trends and conclusions reported throughout this work remain unchanged (Figure ).