Gamma-alumina nanoparticles (γANPs) were obtained from a low-cost process by using natural bauxites. The γANPs materials were characterized by X-ray powder diffraction (XRPD), Fourier-transform infrared spectroscopy (FTIR), Brunauer–Emmett–Teller (BET) theory, scanning electron microscopy (SEM), atomic force microscopy (AFM), and were functionalized with N-cetyl-N, N, N, trimethylammonium bromide (CTAB), leading to CTAB modified γ-alumina nanoparticles (γANPs-CTAB). These novel functionalized γANPs-CTAB were characterized by XRPD, FTIR, and were used as an adsorbent for bisphenol-A (BPA) removal from water. Batch investigations were conducted under different experimental conditions (e.g., adsorbent dose, agitation time, initial concentration, and pH and surfactant loading) in order to optimize BPA adsorption and to identify the adsorption mechanisms in the system γANPs-CTAB-BPA. The effect of pH on the adsorption showed that the quantity of BPA removed increased remarkably until the pH value was 4, then remained almost constant until the pH value was up to 10, and then decreased for pH values greater than 10. For an initial BPA concentration of 20 mg/L and an adsorbent dose of 12.5 g/L at a pH value of 10, the removal efficiency achieved was 91.80 ± 0.21%. The adsorption mechanism was perfectly described by pseudo-second-order kinetics and the Langmuir isotherm. γANPs-CTAB materials were found to be effective adsorbents for BPA removal from water.