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The exploration of highly efficient noble-metal-free catalysts for overall water splitting is crucial for industrial application. In this study, FeS nanosheets/1T-MoS2 nanoflowers on conductive iron foam (IF) were prepared as efficient electrocatalysts for the HER and OER using a solvothermal method. The prepared FMS0.5 electrocatalyst can deliver a high current density of 100 mA cm−2 at low overpotential potentials of 245 and 316 mV and small Tafel slopes of 80.6 and 88.3 mV dec−1 for the HER and OER. The FMS0.5//FMS0.5 exhibited a low voltage of 1.56 V at 10 mA cm−2 with remarkable stability for 40 h in alkaline water. Benefiting from the 3D morphology and interface coupling interactions between the FeS nanosheets and 1T-MoS2 nanoflowers, the self-supporting electrocatalyst could tune the charge/ion transfer path and electronic structure to facilitate the HER and OER activity. Hence, this study would provide new ideas for exploiting highly active non-noble-metal bifunctional catalysts for energy-related applications. [ABSTRACT FROM AUTHOR]