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MgVCr alloys can be considered as alternatives to the TiVCr BCC (body-centered cubic) alloys for hydrogen storage at room temperature, but their synthesis has not been successful so far because Mg is immiscible in V and Cr. In this study, the first MgVCr BCC alloys were synthesized from elemental powders by severe plastic deformation via the high-pressure torsion (HPT) method as well as by high-energy ball milling. Structural homogeneity, thermal stability and hydrogen storage at room temperature were dependent on the composition and the best performances were achieved for the MgVCr composition with the maximum configurational entropy.