A series of ZnFe2O4/expanded graphite composites (EG/ZF) were prepared by the chemical precipitation method. The structure, composition and morphology of the as-prepared samples were characterized. Taking methylene blue (MB) as the simulate organic pollutant, the influences of various factors on the decontamination of the as-samples and their reusing performance were researched. The results showed that the decontamination activity of the EG/ZF composite with mass ratio of EG to ZF equal to 0.8 reaches the maximum in the MB solution of pH = 5, and has good performance for repeated use. What’s more, the possible mechanism of decontamination was studied further.