In this study, an experimental platform for cryo-adsorption and hydrogen storage systems was constructed to investigate the cryo-adsorption hydrogen storage law in the system and explore the kinetic and thermodynamic properties of cryo-adsorption hydrogen storage and the hydrogen storage performance of the entire system. The experimental results demonstrated that the adsorbent material exhibited an excellent hydrogen storage capacity under liquid nitrogen temperature zone conditions, and the adsorbent material demonstrated a high hydrogen storage capacity reaching mass-weight ratio of 5.02%, equivalent to the total hydrogen storage density of 16.63 kg/m³ under a charging pressure of 5 MPa and final storage pressure of 3.04 MPa. Through experimental research, the key factors affecting the hydrogen storage performance were revealed. These factors include the microstructural properties of the adsorbent materials, thermodynamic effects during the adsorption process, and experimental operating conditions. This experimental basis provides a foundation for optimizing the performance of hydrogen storage systems.