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Uniquely structured CoS/N‐doped carbon@MoS2 (denoted as CoS/NC@MoS2) hollow spheres were successfully synthesized by using a well‐designed N‐rich Co‐metal organic framework (ZIF‐67) precursor and template. Owing to the good mechanical stability and conductivity of carbon hollow spheres, N‐doped carbon, and Co−Mo bonds, the as‐prepared CoS/NC@MoS2 composites exhibit outstanding electrochemical performance both in electrocatalytic and energy storage applications. An overpotential of 77 mV at 10 mA cm−2, and a Tafel slope of 67 mV dec−1 could be obtained in acid environment for the hydrogen evolution reaction. As an anode material for lithium‐ion batteries, the as‐prepared composites exhibit good cycling stability with a high reversible specific capacity of 802.4 mA h g−1 at a current density of 1 A g−1 after 400 cycles and good rate capability.

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