The hybrid hydrogen storage method consists of the combination of both solid-state metal hydrides and gas hydrogen storage. This method is regarded as a promising trade-off solution between the already developed high-pressure storage reservoir, utilized in the automobile industry, and solid-state storage through the formation of metal hydrides. Therefore, it is possible to lower the hydrogen pressure and to increase the hydrogen volumetric density. In this work, we design a non-stoichiometric AB2 C14-Laves alloy composed of (Ti0.9Zr0.1)1.25Cr0.85Mn1.1Mo0.05. This alloy is synthesized by arc-melting, and the thermodynamic and kinetic behaviors are evaluated in a high-pressure Sieverts apparatus. Proper thermodynamic parameters are obtained in the range of temperature and pressure from 3 to 85 °C and from 15 to 500 bar: ΔHabs. = 22 ± 1 kJ/mol H2, ΔSabs. = 107 ± 2 J/K mol H2, and ΔHdes. = 24 ± 1 kJ/mol H2, ΔSdes. = 110 ± 3 J/K mol H2. The addition of 10 wt.% of expanded natural graphite (ENG) allows the improvement of the heat transfer properties, showing a reversible capacity of about 1.5 wt.%, cycling stability and hydrogenation/dehydrogenation times between 25 to 70 s. The feasibility for the utilization of the designed material in a high-pressure tank is also evaluated, considering practical design parameters.