A facile strategy was designed to prepare magnetically layered chalcogenide Fe3O4/KMS-1 (FK) composite adsorbents combining the advantages of rapid magnetic separation and satisfactory adsorption performance under vigorous stirring in ethanol solution at room temperature. The dispersion degree of Fe3O4 in ethanol was superior to that in water, which gave a better result with the preparation in ethanol. Characterization by SEM-EDS, XRD, magnetic test, N2 physical-adsorption and TG-DTG demonstrated formation of FK and its adsorption performance. The results showed that the Fe3O4 microspheres could be well distributed over the surface of KMS-1 by electrostatic attraction in ethanol and the obtained FK could be easily separated from water after adsorption using a magnet. The pH slightly affected the adsorption capacity in the range of 3 to 6. Both KMS-1 and Fe3O4 retained their own original adsorption capacity in FK and FK0.3 was the best composite adsorbent when the mass ratio of Fe3O4 and KMS-1 was 0.3. As the amount of loaded Fe3O4 was decreased, the adsorption capacity of the composite adsorbents increased. The kinetic data of FK0.3 fit well with pseudo-second-order models. The co-existing ions had a slight effect on the removal of Zn(II) by FK0.3. The interlayer spacing of KMS-1 in FK increased from 0.851 nm to 1.123 nm after adsorption. The FK composite adsorbents can be considered as an excellent recoverable adsorbent in the treatment of wastewater.