Density functional theory (DFT) calculations were conducted to understand how and why MoS 2 QDs and Mo doping impact the HER and OER activity of NiFeCo-LDHs. To achieve this, we studied how the HER/OER thermodynamics depend on the Ni/Fe/Co ratio, nature of the active site, Mo doping, and MoS 2 -QD deposition using the structures shown in Figure . The activity was quantified by computing the reaction thermodynamics under alkaline reaction conditions using the computational hydrogen electrode method and by studying the electronic structure properties.