In this work, pure nanostructured Mg(2)FeH(6) is successfully synthesized by sintering of a mixture of 2Mg + Fe nanoparticles. The successful preparation of pure Mg(2)FeH(6) can be attributed to the small particle sizes of Mg and Fe nanoparticles prepared by hydrogen plasma-metal reaction (HPMR), which benefits the synthesis. The hydrogen storage properties of Mg(2)FeH(6) and the synthesis mechanism of the Mg-Fe-H system are studied. The sample desorbs 5.0 wt% of hydrogen rapidly in 6 min under an initial hydrogen pressure of approximately 100 Pa at 623 K. The enthalpy and entropy of the reaction are deduced from the equilibrium plateau pressures of the desorption isotherms. The obtained Mg(2)FeH(6) shows favorable hydrogen storage properties due to the specific nanostructure of the materials.