Development of efficient electrocatalysts for complete water splitting is crucial for sustainable hydrogen production. Here, we report a highly active composite of FeMn-layered double hydroxide (LDH) with molybdenum disulfide (MoS2) that exhibits significantly enhanced electrochemical water-splitting activity. The synergistic combination of FeMn-LDH and MoS2 yields improved oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) performances with an overpotential of 222 mV (OER) and 120 mV (HER) at a current density of 10 mA/cm2, respectively. The kinetics study of FeMn-LDH and FeMn-LDH/MoS2 was analyzed with the help of Tafel slopes of 33.35 mV/dec for the OER process and 112 mV/dec for the HER process. The electrocatalyst was stable in both acidic and basic media for more than 24 h. The overall electrocatalysis of water was carried out using two-electrode systems (both electrodes as FeMn-LDH/MoS2 composites) having a low voltage of 1.64 V for a 10 mA cm–2 current density. The enhanced activity is attributed to the increased surface area, improved charge transfer, and modified electronic structure. This work demonstrates a promising strategy for designing efficient electrocatalysts for complete water splitting and sheds light on the potential of LDH/MoS2 composites for energy applications.