carbon, [1] expanded graphite (EG), carbon nanotubes (CNTs), and graphene), dielectric loss materials (ZnO [2] and BaTiO 3), and magnetic loss materials (MFe 2 O 4 , [3] Fe, Co, Ni, and their alloys [4,5]) are generally included. Among them, ferrite materials are widely used as EAMs because of their abundant raw materials, low cost, easy preparation, nontoxicity, and good chemical stability. [3,6] However, their low permittivity and large density render them too thick and heavy to be used in light and thin electronic devices. Besides, EG consisting of sheet-like graphite as an EAM has also attracted much attention. Its excellent properties (low cost, low density, large conductivity, large specific surface area, good antioxidation ability, and big shape anisotropy [6,7]) make it a superb host for nanoparticles. [8] Nevertheless, studies have demonstrated that EG solely used as an EAM hardly meets the high demand of broadband EAMs due to its single conductivity loss and poor impedance matching. Layered C/ferrite nanoparticle array (NPA) and expanded graphite (EG)/C/MFe 2 O 4 (M = Fe, Co, Ni, Zn) NPA heterostructures are synthesized via a simple sodium salt-template method. An array of well-distributed ferrite nanoparticles supported by layered carbon grows simultaneously on the EG surface from metal-oleate complexes. Some dynamic factors are systematically optimized to well adjust the size, content, and morphology of the heterostructures. The heterostructures show good soft magnetic nature with the M s decreasing in the following order: EG/C/γ-Fe 2 O 3 > EG/C/CoFe 2 O 4 > EG/C/NiFe 2 O 4 > EG/C/ZnFe 2 O 4. As microwave absorbers, these heterostructures of EG/C/MFe 2 O 4 NPA exhibit significantly enhanced electromagnetic-wave absorbing capabilities (EWACs) compared with pure EG, EG/γ-Fe 2 O 3 NPA heterostructure, and other C-based composites. Hereinto, EG/C/CoFe 2 O 4 NPA heterostructures exhibit the optimal EWAC with a minimal reflection loss of −49.85 dB at 13.9 GHz and a 1.3 mm coating thickness. The frequency range of 99% absorption is over 2.0-17.0 GHz and the corresponding thickness is 1.10-8.0 mm. The excellent microwave absorption relies on cooperation of double dielectric relaxations, natural resonance, eddy current loss, high attenuation, and appropriate impedance matching. Therefore, layered heterostructures of EG/C/MFe 2 O 4 NPA are promising electromagnetic wave absorbers for practical application.