Microporous organic polymers have special structures and important properties, but their hard processability severely limits their practical applications. In this study, we synthesize nitrogen-containing microporous organic polymer nanofilms by using an interfacial polymerization strategy and then use them as a template to fabricate novel nitrogen-doped microporous carbon nanofilm/molybdenum disulfide (NMC-nanofilm@MoS₂) composites. Owing to the surfaces of NMC nanofilms homogenously covered by MoS₂ nanosheets to form an alternating layer-by-layer nanostructure of MoS₂ and NMC nanofilms, the obtained composite-based electrodes exhibit superior electrochemical performances to the previously reported MoS₂-based composites, with a specific capacity of as high as 1190 mA h g⁻¹ after the 500^th cycle at a current density of 1.0 A g⁻¹, and 908 mA h g⁻¹ after the 2000^th cycle at a current density of 2.0 A g⁻¹.