Because aniline is a persistent pollutant, a cost‐effective and efficient removal method is urgently needed. This study evaluates the synergistic effect of nickel doping in spinel zinc ferrite to enhance the photocatalytic performance of magnetic nanoparticles. Herein, X‐ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), Brunauer–Emmett–Teller (BET), differential reflectance spectroscopy (DRS), transmission electron microscopy (TEM), field emission scanning electron microscopy (FESEM), energy‐dispersive X‐ray spectroscopy (EDX)/Map, and vibrating‐sample magnetometry (VSM) techniques were used to evaluate Ni0.25Zn0.75Fe2O4 MNPs synthesis by a sol–gel method. The produced nanoparticles have a surface area of 20.325 m2 g−1. At room temperature, the nanoparticles exhibit superparamagnetic characteristics and can be readily separated from the aqueous solution. The bandgap has been determined to be 1.83 eV using Tauc's plot. In addition, the photocatalytic activity of as‐prepared Ni0.25Zn0.75Fe2O4 MNPs for aniline degradation under visible light irradiation was examined. The photocatalytic results demonstrate that nickel‐doped zinc ferrite has high photocatalytic activity in aniline degradation. Additionally, Ni0.25Zn0.75Fe2O4 magnetic nanoparticles (MNPs) are highly magnetic in nature, which simplifies separation and repetitive reuse.