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We are reporting the synthesis, the physicochemical, and the hydrogen sorption properties of a novel <i>bcc</i> high entropy alloy Ti_0.30V_0.25Cr_0.10Zr_0.10Nb_0.25. At room temperature, the alloy rapidly absorbs hydrogen reaching a capacity of 2.0 H/M (3.0 wt.%) and forming a dihydride with <i>fcc</i> structure, as confirmed by both synchrotron X-ray diffraction and neutron diffraction. The absorption Pressure–Composition Isotherms corroborated with synchrotron X-ray diffraction prove that the reaction with hydrogen occurs within two steps, i.e., <i>bcc</i> alloy → <i>bcc</i> monohydride → <i>fcc</i> dihydride. The thermodynamic parameters calculated for the second step transformation evidence the formation of a stable dihydride with ΔH<i>_abs</i> = −75 kJ/molH₂. The phase transition during hydrogen/deuterium desorption was investigated by in situ synchrotron X-ray and neutron diffraction confirming a reversible reaction with hydrogen. Furthermore, the cycling properties show a decrease of the capacity over the first cycles followed by a stabilization at 2.44 wt.%, whereas the absorption kinetics improve after the first cycle reaching full capacity after only 30 s at room temperature.