This article introduces a novel iron-cobalt phosphide nanoframe (Fe-CoP NFs) as a bifunctional electrocatalyst for overall water splitting. Fe-CoP NFs, synthesized through a template method involving oriented self-assembly of CoFe PBA precursors followed by mild phosphating, exhibit exceptional performance in both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). The unique nano-framework structure of Fe-CoP NFs provides abundant accessible active sites, reduces kinetic energy barriers, and enhances *O-containing intermediate adsorption, leading to low overpotentials of 255 mV for OER and 122 mV for HER at 10 mA cm$^{-2}$. For overall water splitting, Fe-CoP NFs achieve a cell voltage of 1.65 V, significantly lower than that of conventional nanocubic structures. The catalyst maintains stable performance over 100 hours, outperforming noble metal references. The study highlights the advantages of Fe-CoP NFs in terms of structure, composition, and catalytic activity, demonstrating their potential as efficient, earth-abundant catalysts for water splitting. The findings suggest that hollow structures and appropriate doping can enhance catalytic performance, offering promising prospects for the development of multifunctional materials for sustainable energy applications.This article introduces a novel iron-cobalt phosphide nanoframe (Fe-CoP NFs) as a bifunctional electrocatalyst for overall water splitting. Fe-CoP NFs, synthesized through a template method involving oriented self-assembly of CoFe PBA precursors followed by mild phosphating, exhibit exceptional performance in both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). The unique nano-framework structure of Fe-CoP NFs provides abundant accessible active sites, reduces kinetic energy barriers, and enhances *O-containing intermediate adsorption, leading to low overpotentials of 255 mV for OER and 122 mV for HER at 10 mA cm$^{-2}$. For overall water splitting, Fe-CoP NFs achieve a cell voltage of 1.65 V, significantly lower than that of conventional nanocubic structures. The catalyst maintains stable performance over 100 hours, outperforming noble metal references. The study highlights the advantages of Fe-CoP NFs in terms of structure, composition, and catalytic activity, demonstrating their potential as efficient, earth-abundant catalysts for water splitting. The findings suggest that hollow structures and appropriate doping can enhance catalytic performance, offering promising prospects for the development of multifunctional materials for sustainable energy applications.