This study introduces a computational design approach to create non-metal organic frameworks (NMOFs) from porous organic ammonium halide salts. By combining chemical knowledge with computational crystal-structure prediction (CSP), the researchers designed and synthesized NMOFs that exhibit high ionic charge density and permanent porosity. The key insight is that the nodes in these salt frameworks are tightly packed ionic clusters, which guide the materials to crystallize in specific ways. CSP was used to predict the energy landscapes of these salts, revealing well-defined spikes of low-energy, low-density isoreticular structures. This allowed the selection of cation-anion combinations that form thermodynamically stable, porous salt frameworks with predictable channel sizes, functionalities, and geometries. Some of these porous salts, such as TAPTCl, TTBrCl, and TTBTCl, show high adsorption capacities for molecular guests like iodine, outperforming many metal-organic frameworks (MOFs) in terms of iodine capture. The synthesis of these salts is scalable and involves simple acid-base neutralization, making it possible to create a family of NMOFs with unique properties. The study highlights the potential of NMOFs for applications such as gas capture, catalysis, and molecular separations, and demonstrates the feasibility of designing non-metal organic frameworks using a computational approach.This study introduces a computational design approach to create non-metal organic frameworks (NMOFs) from porous organic ammonium halide salts. By combining chemical knowledge with computational crystal-structure prediction (CSP), the researchers designed and synthesized NMOFs that exhibit high ionic charge density and permanent porosity. The key insight is that the nodes in these salt frameworks are tightly packed ionic clusters, which guide the materials to crystallize in specific ways. CSP was used to predict the energy landscapes of these salts, revealing well-defined spikes of low-energy, low-density isoreticular structures. This allowed the selection of cation-anion combinations that form thermodynamically stable, porous salt frameworks with predictable channel sizes, functionalities, and geometries. Some of these porous salts, such as TAPTCl, TTBrCl, and TTBTCl, show high adsorption capacities for molecular guests like iodine, outperforming many metal-organic frameworks (MOFs) in terms of iodine capture. The synthesis of these salts is scalable and involves simple acid-base neutralization, making it possible to create a family of NMOFs with unique properties. The study highlights the potential of NMOFs for applications such as gas capture, catalysis, and molecular separations, and demonstrates the feasibility of designing non-metal organic frameworks using a computational approach.