Akbari, Sina SadighKaradaş, Ferdi2021-03-012021-03-012020-111864-5631http://hdl.handle.net/11693/75682The development of earth‐abundant photocatalytic assemblies has been one of the bottlenecks for the advancement of scalable water splitting cells. In this study, a ZnCr layered double hydroxide and a CoFe Prussian blue analogue are combined to afford an earth‐abundant photocatalytic assembly involving a visible light‐absorbing semiconductor (SC) and a water oxidation catalyst (WOC). Compared to bare ZnCr‐LDH, the SC‐WOC hybrid assembly exhibits a threefold enhancement in photocatalytic activity, which is maintained for 6 h under photocatalytic conditions at pH 7. The band energy diagram was extracted from optical and electrochemical studies to elucidate the origin of the enhanced photocatalytic performance. This study marks a straightforward pathway to develop low‐cost and precious metal‐free assemblies for visible light‐driven water oxidation.EnglishLayered double hydroxidesPhotocatalysisPrussian blueWater oxidationWater splittingArticle10.1002/cssc.202002279