Evidence shows that embedding metal-based hybrid into carbon matrix is an up-and-coming method to improve the efficiency and decrease the cost of electrocatalysts. Herein, by using a metal-organic framework (MOF) with 4,4-bipyridine and 2,5-thiophenedicarboxylic acid as a precursor, a CoP/Co3S4 hybrid embedded into N, S, O-doped carbon sheets (CoP/Co3S4@NSOC) was constructed through pyrolysis and phosphorization processes. The lamellar morphology, hetero-atom doping, and graphite carbon were favorable for fast electron and mass transfer. Moreover, the strong intrinsic activities of CoP and Co3S4 promoted electrocatalytic performance. In the electrochemical experiments, CoP/Co3S4@NSOC showed the lowest overpotential of 132 [email protected] mA cm−2 for hydrogen evolution reaction (HER) among all the precursors. In addition, the electrocatalytic activity and structure of CoP/Co3S4@NSOC exhibited long-term stability over 60 h. The present work provides a feasible strategy for the construction of robust MOF-derived electrocatalysts.