MgH2　as　one　of　potential　solid-state　hydrogen　storage　materials　has　been　widely　investigated　during　past　decades　due　to　its　large　capacity　and　abundant　elemental　reserves.　Nonetheless,　the　presented　ultra-high　thermal　stability　and　sluggish　kinetics　hinder　a　further　application.　In　the　present　work,　the　Ni　and　Pt　nano-clusters　evolved　from　Ni@Pt　core-shell　nanoparticles　facilitated　the　de/re-hydrogenation　process　of　MgH2.　The　onset　dehydrogenation　temperature　of　MgH2-10　wt%　Ni@Pt　was　greatly　lowered　by　maximum　108　K　compared　with　601　K　of　the　pristine　MgH2,　and　the　dehydrogenation　process　can　be　terminated　below　573　K.　The　thermal　stability　of　the　MgH2-based　system　was　remarkably　tailored　to　69.4　kJ　(mol　H-2)(-1)　from　76.2　kJ　(mol　H-2)(-1)　of　the　pristine　MgH2.　Meanwhile,　the　hydrogen　storage　kinetics　of　MgH2-10　wt%　Ni@Pt　was　greatly　improved　compared　with　the　pristine　MgH2.　Density　functional　theory　calculations　confirmed　that　Pt　nano-clusters　serving　as　a　destabilizer　and　catalyst　not　only　greatly　destabilize　the　thermal　stability　of　MgH2　but　also　catalyze　its　reactions,　in　particular　with　the　Pt(2　2　0)　slab.　The　effective　catalyst-reactant　interfaces　coupling　with　regulated　surface　determined　desorption/absorption　were　deeply　investigated　and　built,　leading　to　an　excellent　agreement　with　experiments.　The　involving　of　transition　metal　clusters　lays　foundation　of　a　new　way　of　improving　the　hydrogen　storage　properties　and　paves　a　way　of　developing　next-generation　hydrogen　storage　materials.