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AbstractToday, around 20% of the electric consumption is devoted to refrigeration, while around 50% of the final energy is dedicated to heating applications. In this scenario, many cooling devices and heat‐pumps are transitioning towards the use of CO2 as an eco‐friendly refrigerant, favouring carbon circular economy. Nevertheless, CO2 still has some limitations, such as large operating pressures (70‐150 bar) and a critical point at 31 °C, which compromise efficiency and increase technological complexity. Very recently, we have reported an innovative breathing‐caloric mechanism in the MIL‐53(Al) compound, which implies gas adsorption under CO2 pressurization boosted by structural transitions, and which overcomes the limitations of stand‐alone CO2. Here, we report the breathing‐caloric‐like effects of MOF‐508b, surpassing by 40% those of MIL‐53(Al). Moreover, we present the first thermometry device operating at room temperature and under the application of only 26 bar of CO2. Under those conditions, our material presents values of ΔT ∼ 30 K, reaching heating temperatures of 56 °C and cooling temperatures of ‐10 °C, which are already useful for space heating, air‐conditioning, food refrigeration and freezing applications.This article is protected by copyright. All rights reserved