Classical Grand Canonical Monte Carlo (GCMC) simulations are performed using the RASPA software to calculate the adsorption uptake of carbon dioxide and nitrogen within MOF structures at 1 bar. GCMC is a well-established method for simulating gas adsorption in porous materials. In this study, GCMC simulation data is regarded as the benchmark for evaluating the adsorption loading in MOFs. Non-bonded interactions are represented by the Lennard-Jones (LJ) potential with a cut-off radius of 12 Å, while Coulomb interactions are calculated using the Ewald summation method with a relative error of 10 -6 . LJ potential parameters for framework atoms are provided by the Universal Force Field (UFF) ; all LJ parameters are listed in Table of the Supplemental Information (SI). Cross-interaction parameters are estimated using the Lorentz-Berthelot combining rules (details in the SI). The partial atomic charges of the structures are calculated using the PACMOF package (), a machine-learning-based model trained on the Density Derived Electrostatic and Chemical (DDEC) partial charges in MOFs . All MOF structures are considered to be rigid. Each uptake point corresponds to a simulation with 10 4 initialization cycles and 10 4 cycles to sample the equilibrium properties.