Designing electromagnetic wave absorption (EMWA) materials with wide bandwidth, strong absorption, and light weight is still a great challenge for practical applications. Herein, the novel nitrogen doped carbon (NDC)/MoS2 composite with rationally designed composition and structure was developed. The NDC particles were introduced into MoS2 nanosheets through the calcination of ZIF-8 precursor and consequent hydrothermal process. A series of characterizations were carried out to investigate the physical properties of the as-prepared nanocomposites. The NDC particles exhibited the shape of rhombic dodecahedron with the size of about 500 nm, which were decorated on flower-shaped MoS2 with the size of about 3 μm. With the increasing NDC content, the absorbing properties of NDC/MoS2 composites increased firstly and then decreased. The features of NDC/MoS2 composite including interconnected porous structure, nitrogen dopant, and appropriate electrical conductivity gave rise to the polarization, multiple reflection, multiple scattering, and impedance matching, resulting in the outstanding EMWA performance. With a filler loading ratio of 30 wt.%, the optimized EMWA property can be achieved when the mass ratio of NDC to MoS2 was adjusted to be 1:1. At a coating thickness of 3.0 mm, the effective EMWA bandwidth (< −10 dB) reached 6.08 GHz (8.56–14.64 GHz). These satisfactory achievements provide a way for the reasonable design of high-performance EMWA and new ideas for future research on wideband EMWA.