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Surface engineering is known as an effective strategy to enhance the catalytic properties of Pt-based nanomaterials. Herein, we report on surface engineering Ni-Pt nanoalloys with a facile method by varying the Ni doping concentration and oleylamine/oleic- acid surfactant-mix. The alloy-composition, exposed facet condition, and surface lattice strain are, thereby manipulated to optimize the catalytic efficiency of such nanoalloys for methanol oxidation reaction (MOR). Exemplary nanoalloys including Ni0.69Pt0.31 truncated octahedrons, Ni0.45Pt0.55 nanomultipods and Ni0.20Pt0.80 nanoflowers are thoroughly characterized, with a commercial Pt/C catalyst as a common benchmark. Their variations in MOR catalytic efficiency are significant: 2.2 A/mgPt for Ni0.20Pt0.80 nanoflowers, 1.2 A/mgPt for Ni0.45Pt0.55 nanomultipods, 0.7 A/mgPt for Ni0.69Pt0.31 truncated octahedrons, and 0.6 A/mgPt for the commercial Pt/C catalysts. Assisted by density functional theory calculations, we correlate these observed catalysis-variations particularly to the intriguing presence of surface interplanar-strains, such as {111} facets with an interplanar-tensile-strain of 2.6% and {200} facets with an interplanar-tensile-strain of 3.5%, on the Ni0.20Pt0.80 nanoflowers.