With the advantages of a long lifetime and high reliability, gas gap heat switches (GGHSs) are attractive in many thermal management applications, especially in space-borne cryogenic systems. The performance of a GGHS is significantly affected by the adsorption characteristics of the adsorbent in the sorption pump. Compared with the commonly used adsorbent in the GGHSs (activated carbon), metal−organic frameworks (MOFs) have larger surface areas, higher pore volumes, and exceptional tunability, which motivates this study to explore their potential for application in cryogenic GGHSs. To this end, two performance metrics, the required volume of adsorbent (v sor ) and total input heat (q tot ), were computed for about 6000 MOFs via molecular simulations and compared with those of activated carbon. It is found that over 2300 MOFs possess a smaller v sor than activated carbon, and the smallest v sor of MOFs is about 12.7% of that of activated carbon. v sor and q tot generally change in the same direction, which implies it is possible to reduce both parameters simultaneously by choosing a suitable MOF. Structure− performance analysis reveals that 1/v sor consistently increases first and then decreases with pore limiting diameter, largest cavity diameter, available pore volume, accessible surface area, helium void fraction, and bulk density. Descriptor ranges corresponding to high-performing MOFs were identified based on Precision-Recall analysis. Notably, Zr-containing MOFs are particularly likely to have smaller v sor values than activated carbon. It is anticipated that the promising MOFs identified by this study will motivate further experimental investigations, and the insights into structure−performance relationships can serve to guide the rational design of novel MOF candidates for GGHSs.