In this research, the performance of PANI@γ-Al2O3 nanocomposite as a new and efficient adsorbent for the removal of Tartrazine dye from water sources was considered. PANI@γ-Al2O3 nanocomposite was characterized by X-ray diffraction, energy-dispersive X-ray, infrared spectroscopy, Field emission scanning electron microscopy, Transmission electron microscope, and Brunauer–Emmett–Teller analyses. The synthesized adsorbent is dumbbell-shaped with two open holes, which causes increases the removal percent of dye. Effective factors including temperature (T), initial dye concentration (Ci), and the adsorbent dosage (m) were recognized by the Plackett–Burman design. A Doehlert design (DD) was applied to optimize the removal conditions of Tartrazine dye. The optimal conditions were obtained as T = 44 °C, Ci = 462.7 mg.L−1 , and m = 0.017 g. The equilibrium adsorption isotherms and kinetic models were also studied. The models of pseudo-second-order kinetics and Freundlich isotherm described the adsorption process well. The maximum uptake capacity (qmax) was 503.1 mg.g−1.