The increasing demand of renewable energy, and the desire to reduce atmospheric levels of CO2, require efficient catalysts for energy conversion processes. Electrochemical water splitting to generate O2 and H2 – where the goal is to use the released electrons to drive CO2 electroreduction – offers a path to a closed “net-zero” emission cycle. Amongst the most active catalysts for the sluggish anode half reaction, the oxygen evolution reaction (OER), are binary combinations of mixed Ni-Fe electrocatalysts. The OER activity on well-defined oxide surfaces such as Ni-Fe nanoparticles have so far not been extensively explored. Here we present a path to highly crystalline Ni-Fe nanocatalysts extended to the series of 3dtransition metals.