Through solar, wind, or geothermal reallocation sources, heat transformation via adsorption-based systems provides the means to address the high energy global demand from refrigeration and cooling. However, improvements toward a suitable, high performing adsorbent−refrigerant working pair must be made to boost the applicability of such systems. For the first time, a series of mesoporous metal−organic frameworks (MOFs) have been tested for R134a fluorocarbon adsorption for this purpose. Each of the selected MOFs exhibit excellent, reversible R134a adsorption. Among them, NU-1000 provided an exceptional fluorocarbon uptake of ∼170 wt % near saturation, which is among the highest values reported so far for MOFs. Exhibiting appropriate equilibrium isotherm behavior and working capacities as large as 125 wt %, it is evident that mesoporous MOFsespecially those with hierarchical structureare promising candidates for chiller applications. Such high performance materials provide significant potential for the design of future adsorption cooling systems.