At present, there is limited research on the application of fuel cell power generation system technology using solid hydrogen storage materials, especially in hydrogen-assisted two-wheelers. Considering the disadvantages of low hydrogen storage capacity and poor kinetics of hydrogen storage materials, our primary focus is to achieve smooth hydrogen ab-/desorption over a wide temperature range to meet the requirements of fuel cells and their integrated power generation systems. In this paper, the Ti0.9Zr0.1Mn1.45V0.4Fe0.15 hydrogen storage alloy was successfully prepared by arc melting. The maximum hydrogen storage capacity reaches 1.89 wt% at 318 K. The alloy has the capability to absorb 90% of hydrogen storage capacity within 50 s at 7 MPa and release 90% of hydrogen within 220 s. Comsol Multiphysics 6.0 software was used to simulate the hydrogen ab-/desorption processes of the tank. The flow rate of cooling water during hydrogen absorption varied in a gradient of (0.02 + x) m s−1 (x = 0, 0.02, 0.04, 0.06, 0.08, 0.1, 0.12). Cooling water flow rate is positively correlated with the hydrogen absorption rate but negatively correlated with the cost. When the cooling rate is 0.06 m s−1, both simulation and experimentation have shown that the hydrogen storage tank is capable of steady hydrogen desorption for over 6 h at a flow rate of 2 L min−1. Based on the above conclusions, we have successfully developed a hydrogen-assisted two-wheeler with a range of 80 km and achieved regional demonstration operations in Changzhou and Shaoguan. This paper highlights the achievements of our team in the technological development of fuel cell power generation systems using solid hydrogen storage materials as hydrogen storage carriers and their application in two-wheelers in recent years.