Abstract: In this work, nanohollow Zn-Fe2O4 spheres were prepared from ZnCl2, FeCl3.6H2O and ammonium acetate using the hydrothermal method. Then, Zn-Fe2O4@ZnO core-shell structured spheres were synthesized by using immobilization of ZnO nanoparticles on surface of Zn-ferrite spheres via sol-gel rout. Scanning electron microscopy (SEM) images showed that the Zn-Fe2O4 and Zn-Fe2O4@ZnO core-shell structured spheres are made of the spherical shape particles. Results of vibrating sample magnetometer (VSM) reveal that the Zn-Fe2O4 nanoparticles are superparamagnetic, whereas in the form of Zn-Fe2O4@ZnO core-shell structured spheres are not. Photocatalytic activity studies confirmed that as-prepared Zn-Fe2O4@ZnO core-shell structured spheres had excellent photodegrading behavior to methylene blue (MB) compared to pure ZnO nanoparticles. Also Zn-Fe2O4@ZnO core-shell structured spheres due to the magnetic properties of environment can be easily removed. Furthermore, Zn-Fe2O4@ZnO core-shell structured spheres could be also served as convenient recyclable photocatalysts because of their magnetic properties.