In this work, we have developed a facile and modular multistep procedure to synthesize hierarchical LDH-based heterostructure electrocatalysts, MoS 2 @NiFeCo-Mo(doped)-LDH. This synthesis involves the hydrothermal growth of trimetallic NiFeCo-LDH onto a nickel foam substrate, subsequent high-valence metal Mo doping into NiFeCo-LDH, and final electrodeposition of MoS 2 QDs on the LDH. The efficient and controllable approach for functionalizing NiFeCo-LDHs with MoS 2 quantum dots and Mo dopants allowed for a systematic study on the MoS 2 @NiFeCo-Mo(doped)-LDHs. We find that the best MoS 2 @NiFeCo-Mo(doped)-LDH and MoS 2 @NiFeCo-LDH heterostructures exhibit very high activity towards HER and OER under both light irradiation and dark conditions in alkaline media. Both materials were also demonstrated to be highly stable under industrially relevant HER and OER 1A cm -2 current densities, with negligible changes in the potential and performance over 25 hours.