The development of cost-effective, highly efficient and robust multi-functional electrode materials can dramatically reduce the overall cost of electrochemical devices. We here report the controlled synthesis of NiS2/FeS2 nanoparticles encapsulated in N-doped carbon nanorods (NiS2/FeS2/NC) through carbonization and sulfurization of Fe/Ni-based bimetallic metal-organic frameworks. Benefiting from both structural and compositional characteristics, the resulting NiS2/FeS2/NC nanorods possess abundant active sites, high electrical conductivity and rapid mass transfer, thereby delivering 10 and 20 mA cm−2 at overpotential of 172 mV and 231 mV towards the hydrogen evolution reaction and oxygen evolution reaction with robust stability in 1.0 M KOH solution, respectively. When employed as a bifunctional electrocatalyst for overall water splitting, it requires only 1.58 V to deliver a current density of 10 mA cm−2 in 1.0 M KOH, outperforming that of the commercial Pt/C || RuO2. Additionally, lithium-ion batteries tests also show high reversible capacity (718 mA h g−1 at 100 mA g−1) and excellent cycling stability and rate performance. The work in this paper not only provides a promising strategy for designing efficient multi-functional electrode materials with similar morphology and structure, but also can be extended to the synthesis of other mixed metal sulfides for energy conversion and storage.