The development and sharing of computational databases for metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) have significantly accelerated the exploration and application of these materials. Recently, molecular materials have emerged as a notable subclass of porous materials, characterized by their crystallinity, modularity, and processability. Among these, macrocycles and cages stand out as representative molecules. Experimentally discovery of a target molecular material from a vast possibility of structures for defined applications is generally impractical due to high experimental costs. This study presents the most extensive Computation-ready Experimental (CoRE) database of macrocycles and cages (MCD) to date, comprising 7,939 structures. Using the MCD, we conducted simulations of binary CO2/CH4 competitive adsorption under conditions relevant to industrial applications. These simulations established a structure-property-function relationship, enabling the identification of materials with potential for CO2/CH4 separation. Among them, a macrocycle, NDI-Δ, exhibited promising CO2 adsorption capacity and selectivity, as confirmed by gas sorption and breakthrough experiments.
