The present work involves the scale-up and characterization of CPO-27–Ni metal organic framework using a range of experimental techniques aimed at determining equilibrium and kinetic parameters to assess its potential for post-combustion carbon capture. CPO-27–Ni was prepared from its precursors by molecular gastronomy methods in kilogram scale. Adsorption of isotherms of pure CO2 and N2 were obtained for different temperatures on these beads, using a volumetric apparatus and the isotherms were fitted to a dual-site Langmuir model. A series of experiments were then carried out in the volumetric apparatus by dosing a known volume of CO2 and the pressure was monitored with time. The diffusional time constants were then extracted by fitting the series of curves to an isothermal diffusion model. From the time constants, the values of the diffusivities were obtained and compared with the values obtained from first principles correlations, which employed the pore size, and the porosity values from independent mercury porosimetry experiments. The results from the analysis showed that the transport of CO2 in the beads was well described by a combination of Knudsen and viscous diffusion mechanisms. Experiments were also carried out using a zero-length column (ZLC) apparatus by preparing a 10% CO2–He and 10% CO2–N2 mixture. The analysis of the ZLC curves showed that the two different carrier gases had an effect of the long-time slope, indicating the presence of a macropore-controlled diffusion mechanism.