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With the environmental pollution and non‐renewable fossil fuels, it is imperative to develop eco‐friendly, renewable, and highly efficient electrocatalysts for sustainable energy. Herein, a simple electrospinning process used to synthesis Mo2C‐embedded multichannel hollow carbon nanofibers (Mo2C‐MCNFs) and followed by the pyrolysis process. As prepared lotus root‐like nanoarchitecture could offer rich porosity and facilitate the electrolyte infiltration, the Mo2C‐MCNFs delivered favourable catalytic activity for HER and OER. The resultant catalysts exhibit low overpotentials of 114 mV and 320 mV at a current density of 10 mA cm−2 for HER and OER, respectively. Furthermore, using the Mo2C‐MCNFs catalysts as a bifunctional electrode toward overall water splitting, which only needs a small cell voltage of 1.68 V to afford a current density of 10 mA cm−2 in the home‐made alkaline electrolyzer. This interesting work presents a simple and effective strategy to further fabricating tunable nanostructures for energy‐related applications. [ABSTRACT FROM AUTHOR]