Due to the good manipulation of electronic structure and defect, anion regulating should be a promising strategy to regulate the electromagnetic (EM) parameters and optimize the EM wave absorption performances (EMWAPs). In this work, we proposed a facile route for the large-scale production of core@shell structured hollow carbon spheres@MoS_xSe_2−x (x = 0.2, 0.6, and 1.0) multicomponent nanocomposites (MCNCs) through a mild template method followed by hydrothermal process. The obtained results revealed that the designed hollow carbon spheres@MoS_xSe_2−x MCNCs presented the improved sulfur vacancy concentration by regulating the x value from 0.2 to 1.0. The obtained hollow carbon spheres@MoS_xSe_2−x MCNCs displayed the extraordinary comprehensive EMWAPs because of the introduced abundant defects and excellent interfacial effects. Furthermore, the as-prepared hollow carbon spheres@MoS_xSe_2−x MCNCs presented the progressively improved comprehensive EMWAPs with the x value increasing from 0.2 to 1.0, which could be explained by their boosted polarization loss abilities and impedance matching characteristics originating from the enhanced sulfur vacancy concentration. Therefore, our findings not only demonstrated that the anion regulating was a promising method to optimize EM parameters and EMWAPs, but also provided a facile route to design the transition metal dichalcogenides-based MCNCs as the much more attractive candidates for high-performance microwave absorbers.