Magnetically recyclable Zn 0.95Àx Cr 0.05 Mn x Al 2 O 4 nanoparticles were synthesized via hydrothermal and heat treatment techniques. The crystal structure, morphology, and photoelectrochemical and magnetic properties of the samples were characterized by x-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), x-ray energy-dispersive spectroscopy (XEDS), ultraviolet-visible (UV-Vis) spectroscopy, photoluminescence spectra (PL), vibrating-sample magnetometer (VSM), electrochemical impedance spectra (EIS) and transient photocurrent responses, and the photocatalytic activity of the samples were evaluated by the photodegradation of methyl orange (MO) dye under simulated sunlight irradiation. The experimental results show that Zn 0.95Àx Cr 0.05 Mn x Al 2 O 4 nanoparticles possess a cubic spinel structure without impurity phases. Cr and Mn ions are successfully substituted in the lattice site of Zn 2+ and enter the ZnAl 2 O 4 matrix. The morphology of the samples exhibits irregular spherical or ellipsoid particles with small particle size and good dispersion. The average crystallite size and the bandgap decrease with an increase in Mn ion concentration. Meanwhile, the co-doped samples exhibit obvious room-temperature ferromagnetism, the photoluminescence intensity decreases and a luminescence quenching phenomenon occurs. In addition, Zn 0.95Àx Cr 0.05 Mn x Al 2 O 4 nanoparticles exhibit excellent photocatalytic activity and possess better photocatalytic reusability in degradation of MO aqueous solution.