We investigated the effect of the aluminum distribution in the adsorption properties of carbon dioxide in the MFI, MOR, and ITW zeolites. Because of its lack of experimental evidence and theoretical validation, Loẅenstein's rule was not generally imposed, and special attention was paid to the effect of the Al−O−Al linkages. To this end, we first generalized an existing transferable force field for CO 2 adsorption in non-Loẅenstein zeolites. By means of molecular simulations based on this force field, we showed that the carbon dioxide adsorption efficiency in MFI is determined by the number of Al atoms, rather than by their distribution in the framework. This was attributed to the small size of the CO 2 molecules compared to the 3D wide-channel topology of the structure. Conversely, we found that the Al distribution has a higher impact on the heat of adsorption in MOR. Although structures with a very high and very low number of non-Loẅenstein bonds presented significant differences, the bonds themselves do not affect the heat of adsorption directly. Instead, we found that an homogeneous distribution of the Al atoms in the sites forming the C-channel is more favorable. Finally, the small-pore distribution of the ITW zeolite led to high values of the heat of adsorption and wide error bars, which made the study feasible just for low aluminum concentrations. In that case, we report a small dependency of the heat of adsorption on the Al distribution.