This study presents the development of porous, non-metal organic frameworks (CPOS) using computational crystal-structure prediction (CSP). The research demonstrates that porous organic ammonium halide salts can be designed with no metals, leveraging the isoreticular principle to achieve predictable, stable structures. These materials exhibit high ionic charge density and permanent porosity, making them suitable for applications such as gas capture and molecular separations. The study shows that CSP can be used to design these materials by identifying low-energy, low-density isoreticular structures on energy landscapes, which guide the selection of cations and anions to form thermodynamically stable, porous frameworks. The resulting materials can adsorb molecular guests like iodine in quantities exceeding those of many metal-organic frameworks (MOFs), with potential applications in radio-iodine capture. The study also highlights the scalability of the synthesis process, involving simple acid-base neutralization, and the ability to create a family of non-metal organic frameworks with high ionic charge density and permanent porosity. The research underscores the importance of computational methods in designing porous materials and provides insights into the design of non-metal organic frameworks with unique properties. The study also discusses the challenges in designing porous molecular crystals and the potential of CSP in overcoming these challenges. The results demonstrate the feasibility of creating porous organic salts with predictable, isoreticular structures, which could lead to new applications in materials science. The study also highlights the importance of understanding the relationship between crystal structure and physical properties in the design of porous materials. The research provides a framework for the rational design of porous materials and offers new insights into the potential of non-metal organic frameworks in various applications.This study presents the development of porous, non-metal organic frameworks (CPOS) using computational crystal-structure prediction (CSP). The research demonstrates that porous organic ammonium halide salts can be designed with no metals, leveraging the isoreticular principle to achieve predictable, stable structures. These materials exhibit high ionic charge density and permanent porosity, making them suitable for applications such as gas capture and molecular separations. The study shows that CSP can be used to design these materials by identifying low-energy, low-density isoreticular structures on energy landscapes, which guide the selection of cations and anions to form thermodynamically stable, porous frameworks. The resulting materials can adsorb molecular guests like iodine in quantities exceeding those of many metal-organic frameworks (MOFs), with potential applications in radio-iodine capture. The study also highlights the scalability of the synthesis process, involving simple acid-base neutralization, and the ability to create a family of non-metal organic frameworks with high ionic charge density and permanent porosity. The research underscores the importance of computational methods in designing porous materials and provides insights into the design of non-metal organic frameworks with unique properties. The study also discusses the challenges in designing porous molecular crystals and the potential of CSP in overcoming these challenges. The results demonstrate the feasibility of creating porous organic salts with predictable, isoreticular structures, which could lead to new applications in materials science. The study also highlights the importance of understanding the relationship between crystal structure and physical properties in the design of porous materials. The research provides a framework for the rational design of porous materials and offers new insights into the potential of non-metal organic frameworks in various applications.