Five-fold intertwined Ag x Ni 1Àx (x = 0.01-0.25) heterogeneous alloynanocrystal (NC) catalysts,prepared through unique reagent combinations,a re presented. With only ca. 5at% Ag (AgNi-5), Pt-like activity has been achieved at pH 14. To reachacurrent density of 10 mA cm À2 the extremely stable AgNi-5 requires an overpotential of 24.0 AE 1.2 mV as compared to 20.1 AE 0.8 mV for 20 %P t/C,b oth with equal catalyst loading of 1.32 mg cm À2 .T he turnover frequency (TOF) is as high as 2.1 H 2 s À1 at 50 mV (vs.R HE). Sitespecific elemental analyses show the Ag:Ni compositional variation, where the apex and edges of the decahedra are Agrich, therebye xposing Ni onto the faces to achieve maximum charge transport for an exceptional pH universal HER activity. DFT calculations elucidate the relative H-atom adsorption capability of the Ni centers as af unction of their proximity to Ag atom.