Two supramolecular crystals, RP-H100 and RP-H101, were constructed from imidazole-annulated triptycene hexacarboxylic acids, noted as IATH-1 and IATH-2, respectively, into 7-fold catenated network structures. Strikingly, RP-H101 exhibits high gravimetric (3526 m² g^‒1) and high volumetric (1855 m² cm^‒3) surface areas, surpassing all previously reported supramolecular crystals. These exceptional features give record-high hydrogen deliverable capacities among all reported porous materials, with volumetric capacity of 54.6 g L^‒1 and gravimetric capacity of 9.3 wt% under a combined temperature and pressure swing (77 K/100 bar → 160 K/5 bar). This groundbreaking advancement in hydrogen storage highlights the potential of supramolecular crystals and the effectiveness of the point-contact catenation strategy, paving the way for stable, scalable, and processable[8] porous materials for industrial applications.  two supramolecular crystals, RP-H100 and RP-H101, were constructed from imidazole-annulated triptycene hexacarboxylic acids, noted as IATH-1 and IATH-2, respectively, into 7-fold catenated network structures. Strikingly, RP-H101 exhibits high gravimetric (3526 m2 g‒1) and high volumetric (1855 m² cm^‒3) surface areas, surpassing all previously reported supramolecular crystals. These exceptional features give record-high hydrogen deliverable capacities among all reported porous materials, with volumetric capacity of 54.6 g L^‒1 and gravimetric capacity of 9.3 wt% under a combined temperature and pressure swing (77 K/100 bar → 160 K/5 bar). This groundbreaking advancement in hydrogen storage highlights the potential of supramolecular crystals and the effectiveness of the point-contact catenation strategy, paving the way for stable, scalable, and processable[8] porous materials for industrial applications.