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Water electrolysis is an emerging energy conversion technology, which is significant for efficient hydrogen (H2) production. Based on the high‐activity transition metal ions and metal alloys of ultrastable bifunctional catalyst, the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are the key to achieving the energy conversion method by overall water splitting (OWS). This study reports that the Co‐based coordination polymer (ZIF‐67) anchoring on an indium–organic framework (InOF‐1) composite (InOF‐1@ZIF‐67) is treated followed by carbonization and phosphorization to successfully obtain CoP nanoparticles–embedded carbon nanotubes and nitrogen‐doped carbon materials (CoP‐InNC@CNT). As HER and OER electrocatalysts, it is demonstrated that CoP‐InNC@CNT simultaneously exhibit high HER performance (overpotential of 153 mV in 0.5 m H2SO4 and 159 mV in 1.0 m KOH) and OER performance (overpotential of 270 mV in 1.0 m KOH) activities to reach the current density of 10 mA cm−2. In addition, these CoP‐InNC@CNT rods, as a cathode and an anode, can display an excellent OWS performance with η10 = 1.58 V and better stability, which shows the satisfying electrocatalyst for the OWS compared to control materials. This method ensures the tight and uniform growth of the fast nucleating and stable materials on substrate and can be further applied for practical electrochemical reactions.