Cryogenic supercritical hydrogen storage technology is a high-density physical hydrogen storage method, which is a highly promising hydrogen storage approach. However, existing research has mainly focused on the development of storage devices for cryogenic supercritical hydrogen, with limited research on the cooling process of supercritical hydrogen. Therefore, a novel cooling process for cryogenic supercritical hydrogen production based on helium expansion cycle with liquid nitrogen (LN2) pre-cooling is proposed in this paper. In this process, after being compressed and cooled in multiple stages, the feed hydrogen is pre-cooled by LN2. Then, cryogenic supercritical hydrogen (10 MPa, −235.15 °C, 63.36 g/L) is obtained by helium multi-stage expansion refrigeration. The process is simulated by Aspen HYSYS and optimized by genetic algorithm (GA) to obtain lower specific energy consumption (SEC). Thermodynamic analyses are conducted to evaluate the process. And compared with the conventional hydrogen liquefaction process, the results show that the proposed process is reasonable and superior. The SEC0, figure of merit (FOM), and the total exergy loss of the system are 5.432 kWh/kgH2, 43.88%, and 289.69 kW respectively. This study indicates that the proposed process has significant implications for the hydrogen industry and provides valuable information for cryogenic supercritical hydrogen storage systems.