The　development　of　highly　efficient　bifunctional　electrocatalysts　with　excellent　stability　at　high　current　densities　for　overall　water　splitting　is　a　challenging　but　urgent　goal.　Herein,　a　novel　kind　of　significantly　efficient　bifunctional　electrocatalysts　has　been　elaborately　designed　through　the　fabrication　of　Fe-doped　Ni2P　nanosheets　decorated　with　CeO2　nanoparticles　(Fe-Ni2P/CeO2)　grown　on　Ni　foam.　It　reveals　the　existence　of　electron　transfer　from　Ni2+　to　Ce4+,　resulting　in　an　increase　of　Ni3+,　of　which　the　strong　Lewis　acidity　promotes　the　adsorption　of　OH−　and　thus　facilitates　the　formation　and　conversion　of　oxygen-related　intermediates　during　the　water　splitting　process.　The　resulting　catalyst　shows　outstanding　electrocatalytic　activities　for　both　oxygen　evolution　reaction　(OER)　(η20　=　190　mV,　η1000　=　260　mV)　and　hydrogen　evolution　reaction　(HER)　(η20　=　78　mV,　η1000　=　292　mV).　Moreover,　when　utilized　for　overall　water　splitting,　the　Fe-Ni2P/CeO2　requires　very　low　voltages　of　1.52　V　and　2.88　V　to　achieve　current　densities　of　20　mA　cm−2　and　1000　mA　cm−2,　respectively,　outperforming　the　Pt/C　||　RuO2　electrolyzer.　Importantly,　the　as-designed　electrolyzer　exhibits　exceptional　durability　at　a　high　current　density　of　1000　mA　cm−2.　This　work　has　demonstrated　an　effective　strategy　for　designing　non-precious　metal　heterojunctions　with　abundant　electrocatalytic　active　sites　to　drive　efficient　overall　water　splitting.　©　2024　Elsevier　B.V.