Lightweight reduced graphene oxide aerogel (rGO) has obtained enormous attention as microwave absorber due to anisotropic characteristics in their structure and electromagnetic parameters. However, the controllable preparation of reduced graphene oxide (rGO) aerogels with tailored multidimensional structure with broadened effective absorption bandwidth is a thorny difficulty. In this paper, rGO aerogel decorated with molybdenum sulfide (rGO/MoS2) with three-dimensional (3D) layered porous structure were synthesized by a two-step hydrothermal method. The unique three-dimensional layered porous structure of graphene aerogel not only effectively avoids the stacking of graphene flake layers, but also provides space for the loading of MoS2 nanosheets. The introduction of MoS2 nanosheets compensates for the imbalance of impedance matching caused by graphene due to the excessive conductivity, and the folded MoS2 nanosheets are uniformly loaded on the graphene lamellae, which is conducive to generate multiple reflections and scattering of electromagnetic waves. Besides, the construction of heterogeneous interfaces strengthens the interfacial polarizability of the composites. As a result, excellent electromagnetic wave attenuation properties were obtained for rGO/MoS2, and the effective absorption bandwidth (EAB) reached 6.56 GHz at 2.1 mm. In addition, the radar cross section (RCS) simulation results further demonstrate the dissipation capability of the composite in practical application scenarios. This paper provides a new idea for the design of lightweight EM wave absorbing materials with broad absorption bandwidth.