Hydrogen storage is crucial in the shift toward a carbon-neutral society, where hydrogen serves as a pivotal renewable energy source. Utilizing porous materials can provide an efficient hydrogen storage solution, reducing tank pressures to manageable levels and circumventing the energy-intensive and costly current technological infrastructure. Herein, we report two highly porous aromatic frameworks (PAFs), C-PAF and Si-PAF, prepared through a Yamamoto C-C coupling reaction between trigonal prismatic monomers. These PAFs exhibited large pore volumes and BET areas, 3.93 cm3 g-1 and 4857 m2 g-1 for C-PAF, and 3.80 cm3 g-1 and 6099 m2 g-1 for Si-PAF, respectively. Si-PAF exhibited a record-high gravimetric hydrogen delivery capacity of 17.01 wt% and a superior volumetric capacity of 46.5g L-1 under pressure-temperature swing adsorption conditions (77 K, 100bar → 160 K, 5bar), outperforming benchmark hydrogens storage materials. By virtue of the robust C-C covalent bond, both PAFs showed impressive structural stabilities in harsh environments and unprecedented long-term durability. Computational modeling methods were employed to simulate and investigate the structural and adsorption properties of the PAFs. These results demonstrate that C-PAF and Si-PAF are promising materials for efficient hydrogen storage. This article is protected by copyright. All rights reserved.