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Abstract The development of porous materials is of great interest for the capture of CO₂from various emission sources, which is essential to mitigate its detrimental environmental impact. In this direction, porous organic polymers (POPs) have emerged as prime candidates owing to their structural tunability, physiochemical stability and high surface areas. In an effort to transfer an intrinsic property of a cyclotetrabenzoin‐derived macrocycle – its high CO₂affinity – into porous networks, herein we report the synthesis of three‐dimensional (3D) macrocycle‐based POPs through the polycondensation of an octaketone macrocycle with phenazine‐2,3,7,8‐tetraamine hydrochloride. This polycondensation was performed under ionothermal conditions, using a eutectic salt mixture in the temperature range of 200 to 300 °C. The resulting polymers, named 3D‐mmPOPs, showed reaction temperature‐dependent surface areas and gas uptake properties. 3D‐mmPOP‐250 synthesized at 250 °C exhibited a surface area of 752 m² g⁻¹and high microporosity originating from the macrocyclic units, thus resulting in an excellent CO₂binding enthalpy of 40.6 kJ mol⁻¹and CO₂uptake capacity of 3.51 mmol g⁻¹at 273 K, 1.1 bar.