Eriochrome black T is considered as one of the anionic dyes with potential harmful effects on human health and the environment. Among other processes, adsorption can contribute to the removal of these dyes. In the present study, two adsorbent materials, pseudo-boehmite (γ-AlOOH) and gamma alumina (γ-Al2O3), were synthesized and tested in the removal of the Eriochrome black T molecule (EBT). γ-AlOOH and γ-Al2O3 were obtained by precipitation from NaAlO2 solution at pH = 7, at a temperature of 80 °C, and by the thermal transformation of γ-AlOOH at 800 °C, respectively. In order to gain insights into the structural, chemical, thermal and morphological properties of these materials, numerous analytical techniques were involved, including X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), differential thermogravimetric–thermal analysis (TGA-DTA), scanning electron microscopy with energy-dispersive spectroscopy (SEM-EDS), and specific surface area measurement using the Brunauer–Emmett–Teller (BET) method. Several adsorption parameters were studied, such as the adsorbent dose, initial concentration, pH, contact time and reaction temperature. The kinetic study showed that EBT adsorption follows the pseudo-second-order model. The Langmuir isotherm model revealed a maximum EBT adsorption capacity of 344.44 mg g−1 and 421.94 mg g−1 for γ-AlOOH and γ-Al2O3, respectively. A textural and structural analysis after adsorption highlighted the effective adsorption of the dye.