AbstractThe synthesis of hybrid platinum materials is fundamental to enable alkaline water electrolysis for cost‐effective H2 generation. In this work, we have used a galvanostatic method to co‐deposit PtNi films onto polycrystalline gold. The surface concentrations of Ni (ΓNi) and Pt (ΓPt) were calculated from electrochemical measurements; the ΓPt/ΓNi ratio and electrocatalytic activity of these materials towards hydrogen evolution reaction (HER) in 1 M KOH show a strong dependence on the current density pulse applied during the electrodeposition. Analysis of the Tafel parameters hints that, on these deposits, HER proceeds through a Volmer‐Heyrovsky mechanism. The galvanostatically deposited PtNi layers present a high current output per Pt gram, 3199 A gPt−1, which is significantly larger compared to other PtNi‐based materials obtained by more extended and more complex synthesis methods.