The catalytic dehydrogenation of hydrazine borane (N2H4BH3) and hydrous hydrazine (N2H4 center dot H2O) for H-2 evolution is considered as two of the pivotal reactions for the implementation of the hydrogen-based economy. A reduction rate controlled strategy is successfully applied for the encapsulating of uniform tiny NiPt alloy nano clusters within the opening porous channels of MOFs in this work. The resultant Ni0.9Pt0.1/MOF core shell composite with a low Pt content exerted exceedingly high activity and durability for complete H2 evolution (100% hydrogen selectivity) from alkaline N2H4BH3 and N2H4 center dot H2O solution. The features of small NiPt alloy NPs, strong synergistic effect between NiPt alloy NPs and the MOF, and open pore structure for freely mass transfer made NiPt/MIL-101 an excellent catalyst for highly efficient H-2 evolution from N2H4BH3 or N2H4 center dot H2O.