In this study, biopolymer chitosan is presented as a template for synthesizing and shaping the mesoporous γ‐Al2O3 macrospheres. This porous γ‐Al2O3 granule has a high surface area (310 m2/g), high pore volume (.6148 cm3/g), and pore diameter between 2 and 10 nm. The full factorial design based on a mathematical model was implemented to study the acid concentration, chitosan amount, ammonia concentration, and aging time affecting the responses (Brunauer–Emmett–Teller surface area and pore volume). Predicted responses were found to be in satisfactory agreement with experimental values (R2 = .9580 and .9109, respectively). The adequacy of the model was examined by analyzing the residual distribution plots and Pareto graph. X‐ray diffraction, scanning electron microscopy (SEM), thermogravimetric analysis, and N2 adsorption/desorption techniques are employed to characterize the structure of the prepared γ‐alumina sample.