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In the present study Mg2Ni-type compounds alloyed independently with Ti, V, Fe and Si were successfully prepared by wet-milling followed by sintering. Although these alloyed Mg2Ni compounds exhibited a similar hydrogen storage mechanism as that of pure Mg2Ni, the dissolution of Ti, V or Fe into the Mg2NiH4 lattice had a considerable catalytic effect on hydrogen desorption from additional MgH2. The further structure investigations clearly indicated that the substitution of Ti for Ni could suppress the formation of the micro-twined low-tem-perature phase (LT2) and promote the formation of the high-temperature phase (HT), thus resulting in re-markably improved hydrogen desorption kinetics for the Mg2Ni0.92Ti0.08-H system.