The self−assembly among different two−dimensional materials could effectively improve the self−stacking effect and promote repeated reflection and refraction of incident electromagnetic wave (EMW). The polarization effect caused by the heterogeneous contact also helps the attenuation of EMW. In this study, the in−situ hydrothermal approach was used to effectively fabricate petal−like CoFe−layered double hydroxide sheets (CoFe−LDH) grown on reduced graphene oxide (RGO) functionalized by 4,4−diaminodiphenyl methane (DDM). The microwave absorption properties of DDM−functionalized RGO/CoFe−layered double hydroxide composites (DDM−RGO/LDH) were investigated. When the loading of DDM−RGO is 40.0 ​mg, the reflection loss reached −60.0 ​dB at 5.28 ​GHz, resulting in great EMW absorption performance. The effective absorption bandwidth at 2.00 ​mm is 5.28 ​GHz. The results show that DDM−RGO/LDH has a wide microwave absorption bandwidth and strong absorption capability, thus could be applied as an advanced EMW absorbing material.