Abstract: | Herein, we demonstrate the use of heterostructures comprised of Co/β‐Mo2C@N‐CNT hybrids for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in an alkaline electrolyte. The Co can not only create a well‐defined heterointerface with β‐Mo2C but also overcomes the poor OER activity of β‐Mo2C, thus leading to enhanced electrocatalytic activity for HER and OER. DFT calculations further proved that cooperation between the N‐CNTs, Co, and β‐Mo2C results in lower energy barriers of intermediates and thus greatly enhances the HER and OER performance. This study not only provides a simple strategy for the construction of heterostructures with nonprecious metals, but also provides in‐depth insight into the HER and OER mechanism in alkaline solution. |