Electrocatalytic water splitting into H 2 and O 2 is ak ey technology for carbon-neutral energy.H ere,w er eport am odular materials design leading to noble metal-free composite electrocatalysts,w hich combine high electrical conductivity,h igh OER and HER reactivity and high durability.T he scalable bottom-up fabrication allows the stable deposition of mixed metal oxide nanostructures with different functionalities on copper foam electrodes.T he composite catalyst shows sustained OER and HER activity in 0.1m aqueous KOHo verp rolonged periods (t > 10 h) at low overpotentials (OER: % 300 mV; HER: % 100 mV) and high faradaic efficiencies (OER: % 100 %, HER: % 98 %). The new synthetic concept will enable the development of multifunctional, mixed metal oxide composites as high-performance electrocatalysts for challenging energy conversion and storage reactions.Electrocatalytic water splitting into hydrogen and oxygen is one of the most promising catalytic approaches for carbonneutral energy storage. [1][2][3] Theoverall process is based on two coupled electrochemical half-reactions,the oxygen evolution reaction (OER) [4,5] and the hydrogen evolution reaction (HER). [2,6,7] Fori ndustrial relevance,b oth half-reactions require noble-metal-free catalysts,which combine high activity with long-term stability.T herefore,synthetic methods are required for the chemically,m echanically and electrically stable anchoring of high-performance catalysts on conductive electrode surfaces. [1,2,8] State-of-the-art electrocatalysis research has been focused on the independent development of HER and OER catalysts,sothat each half-reaction can be individually optimized. [1][2][3] ForH ER electrocatalysis, [9] the focus has been on homo-or heterometallic transition metal oxides, [10] sulfides, [11] nitrides, [12] carbides, [12] and phosphides. [13] ForO ER, [5] the leading electrocatalysts are homoand heterometallic transition metal oxides, [14,15] hydroxides, [16,17] phosphates, [18] and nitrides. [19] In contrast, the design of bifunctional catalysts capable of OER and HER electrocatalysis is still in its infancy and faces major challenges,asnew catalysts are needed, which feature the redoxchemistries,s tabilities and catalytic capabilities for reductive and oxidative proton-coupled electron transfers.H owever, the design of bifunctional OER/HER electrocatalysts offers vast advantages as it would simplify catalyst design and fabrication, prevent cross-contamination, materials incompatibilities and possible catalyst poisoning and is therefore of enormous technological interest. In addition, HER and OER electrocatalysis share common challenges including the need for high electrical conductivity,t he stable catalyst-electrode anchoring and others,s ot hat ac onvergent OER/HER catalyst design could overcome major current obstacles in electrocatalysis.T od ate,o nly few materials have shown this broad range of properties and most pioneering studies have used metal phosphides such as nickel phosphides, [20] iron nickel phosphides, [6] and ...