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Large-area and flexible reduced graphene oxide (rGO)/Fe3O4 NPs/polyurethane (PU) composite films are fabricated by a facile solution-processable method.The monolayer assembly of Fe3O4 nanoparticles with a high particle-stacking density on the graphene oxide (GO) sheets is achieved by mixing two immiscible solutions of Fe3O4 nanoparticles in hexane and GO in dimethylformide (DMF) by a mild sonication.The x-ray diffraction and Raman spectrum confirm the reduced process of rGO by a simple thermal treatment.The permittivity value of the composite in a frequency range of 0.1 GHz-18 GHz increases with annealing temperature of GO increasing.For 5-wt% rGO/Fe3O4 NPs/PU,the maximum refection loss (RL) of over-35 dB appears at 4.5 GHz when the thickness of film increases to 5 mm.The rGO/Fe3O4 NPs/PU film,exhibiting good electromagnetic properties over GHz frequency range,could be a potential candidate as one of microwave absorption materials in flexible electronic devices.