Excavated cubic Pt93Ir7 alloy nanocrystals enclosed by high-index {710} facets exhibit excellent electrocatalytic properties for the nitrogen reduction reaction (NRR) with a high faradaic efficiency (40.8%) and NH3 production rate (28 μg h-1 cm-2). The presence of Ir on the Pt stepped surface suppresses the hydrogen evolution reaction (HER) and accelerates the NRR.