Supported Fe-doped Pd-nanoparticles (NPs) are prepared via soft transfor-mation of a PdFe-metal oraganic framework (MOF). The thus synthesized bimetallic PdFe-NPs are supported on FeOx@C layers, which are essential for developing well-defined and distributed small NPs, 2.3 nm with 35% metal loading. They are used as bifunctional nanocatalysts for the electro-catalytic water splitting process. They display superior mass activity for the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER), both in alkaline and acid media, compared with those obtained for benchmarking platinum HER catalyst, and ruthenium, and iridium oxide OER catalysts. PdFe-NPs also exhibit outstanding stability against sintering that can be explained by the protecting role of graphitic carbon layers provided by the organic linker of the MOF. Additionally, the superior electrocatalytic performance of the bimetallic PdFe-NPs compared with those of monometallic Pd/C NPs and FeOx points to a synergetic effect induced by Fe-Pd interactions that facilitates the water splitting reaction. This is supported by additional characterization of the PdFe-NPs prior and post electrolysis by TEM, XRD, X-ray photoelectron spectroscopy, and Raman revealing that dispersed PdFe NPs on FeOx@C promote interactions between Pd and Fe, most likely to be Pd-O-Fe active centers.