The bulk mechanical alloying (BMA) is used to make grain size refinement of palladium and to synthesize Mg2Ni in the solid state from the granular mixture. Different from the conventional mechanical alloying by ball-milling or attriting, no hard balls or vials are used in the present processing. Since palladium platelets and magnesium/nickl granules can be used as an input material, no powders are needed in preparation. Comparing the pressure-composition isotherms between normal-sized and nano-sized palladium, the effect of nano-structuring on the hydrogen absorbing behavior is discussed with notes on the induced strains during BMA and the thermodynamic properties. Nano-structured Mg2Ni is synthesized in solid-state to understand the effect of nano-structuring and non-equilibration on the hydrogen storage capacity. Further potentiality of BMA is pointed out as an effective solid-state fabrication of various nano-structured or non-equilibrium phase materials.