Tuning the crystal phase of metal alloy nanomaterials has been proved as ignificant way to alter their catalytic properties based on crystal structure and electronic property. Herein, we successfully developed as imple strategy to controllably synthesize ar are crystal structure of hexagonal close-packed (hcp) NiFen anoparticle (NP) encapsulated in aN -doped carbon (NC) shell (hcp-NiFe@NC). Then, we systemically investigated the oxygen evolution reaction (OER) performance of the samples under alkaline conditions,i n which the hcp-NiFe@NC exhibits superior OER activity compared to the conventional face-centered cubic (fcc) NiFe encapsulated in aN-doped carbon shell (fcc-NiFe@NC). At the current densities of 10 and 100 mA cm À2 ,t he hcp-NiFe@NC with Fe/Ni ratio of % 5.4 %only needs ultralow overpotentials of 226 mV and 263 mV versus reversible hydrogen electrode in 1.0 m KOHe lectrolyte,r espectively,w hich were extremely lower than those of fcc-NiFe@NC and most of other reported NiFe-based electrocatalysts.W ep roposed that hcp-NiFep ossesses favorable electronic property to expedite the reaction on the NC surface,r esulting higher catalytic activity for OER. This researchp rovides an ew insight to design more efficient electrocatalysts by considering the crystal phase correlated electronic property.