The industry development in the last 200 years has led to to environmental pollution. Dyes emitted by pharmaceutical and other industries are major organic pollutants. Organic dyes are a pollutant that must be removed from the environment. In this work, we adopt a facile microwave hydrothermal method to synthesize ZnFe2O4/rGO (ZFG) adsorbents and investigate the effect of synthesis temperature. The crystal structure, morphology, chemical state, and magnetic property of the nanocomposite are investigated by X-ray diffraction, Raman spectroscopy, Fourier transform infrared spectroscopy, transmission electron microscopy, and a vibrating sample magnetometer. Furthermore, the synthesized ZFGs are used to remove methylene blue (MB) dye, and the adsorption kinetics, isotherm, mechanism, and reusability of this nanomaterial are studied. The optimal ZFG nanocomposite had a dye removal percentage of almost 100%. The fitting model of adsorption kinetics followed the pseudo-second-order model. The isotherm model followed the Langmuir isotherm and the theoretical maximum adsorption capacity of optimal ZFG calculated by this model was 212.77 mg/g. The π–π stacking and electrostatic interaction resulted in a high adsorption efficiency of ZFG for MB adsorption. In addition, this nanocomposite could be separated by a magnet and maintain its dye removal percentage at almost 100% removal after eight cycles, which indicates its high suitability for utilization in water treatment.