In this study, NiFe2O4@AC/UiO‐66(Zr) composites were successfully prepared with different ratios of UiO‐66(Zr) as support for NiFe2O4@AC, (1 : 1), (2 : 1) and (3 : 1) named NiFe2O4@AC/UiO‐66(Zr)‐1, NiFe2O4@AC/UiO‐66(Zr)‐2 and NiFe2O4@AC/UiO‐66(Zr)‐3, respectively. The prepared composites were characterized by X‐Ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), X‐Ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), scanning electron microscopy (SEM), Brunauer–Emmett–Teller (BET), ultraviolet‐visible diffuse reflectance (UV‐Vis/DRS) spectroscopy, PL (Photoluminescence) study. The synthesized composites′ efficiencies to enhance the photodegradation of alizarin yellow R (AYR) under visible‐light were evaluated. The results identified that NiFe2O4@AC/UiO‐66(Zr)‐2 is the most photoreactive photocatalyst with the lowest bandgap ∼1.7 eV. NiFe2O4@AC/UiO‐66(Zr)‐2 shows higher photodegradation efficiency (97.9 %) compared to NiFe2O4@AC/UiO‐66(Zr)‐1 and NiFe2O4@AC/UiO‐66(Zr)‐3 with photodegradation efficiency of 75.1 % and 89.9 %, respectively after 180 min under visible‐light. The photodegradation reaction of AYR was found to be pseudo first‐order reaction, and the rate constant (Ka) for NiFe2O4@AC/UiO‐66(Zr)‐1, NiFe2O4@AC/UiO‐66(Zr)‐2, and NiFe2O4@AC/UiO‐66(Zr)‐3 are 0.0072 min−1, 0.0204 min−1, and 0.0122 min−1, consecutively. The effects of various conditions such as initial concentration and photocatalyst dose on the photodegradation of AYR were determined. The high photodegradation efficiency of NiFe2O4@AC/UiO‐66(Zr)‐2 composite is because of the heterojunction and effective charge transfer between NiFe2O4@AC and UiO‐66(Zr). NiFe2O4@AC/UiO‐66(Zr)‐2 photocatalyst exhibits photocatalytic stability and reusability up to five cycles.