We synthesized new composite particles for hydrogen storage on the basis of an idea of "particle designing". As starting materials, powders of Mg and YNi2 were selected. Fine composite particles containing mainly Mg2Ni could be designed by repetitive hydriding and dehydriding cycles at 673 K. In the synthesis process of the composite particles, the following two points were found to be essential for this technique. The first point is that, after being activated by the sequential processes of hydrogenation, amorphization and disproportionation, YNi2 reacts effectively with Mg. The second point is that evaporated Mg, which occurs during dehydriding, adheres to the surface of the activated YNi2 and accelerates a diffusion reaction to form Mg2Ni at the interface. In these composite particles, Mg2NiH4 is formed, even at 373 K, under a hydrogen pressure of 5 MPa.