A series of porous γ-Al₂O₃ materials was prepared by solution-combustion and ball-milling processes. The as-prepared powders were physicochemically characterized by x-ray diffraction (XRD), scanning electron microscopy (SEM), and N₂ physisorption measurements and their performances in CO₂ adsorption at different pressures (0.5 to 1.5 MPa) and temperatures (40 to 60ºC) were investigated. It was found that γ-Al₂O₃ synthesized by the solution-combustion process and ball milled at 10 hr exhibited the best CO₂ adsorption performance at 60ºC and 1.5 MPa, achieving a maximum of 1.94 mmol/g compared to the four studied materials, as a result of their interesting microstructure and surface properties (i.e., nanocrystallinity, specific surface area, narrow pore size distribution, and large total pore volume). Our study shows that the γ-Al₂O₃ prepared by solution combustion followed by ball milling presents a fairly good potential adsorbent for efficient CO₂ capture. Implications: In this work, γ-Al₂O₃ materials were successfully obtained by solution combustion and modified via ball milling. These improved materials were systematically investigated as solid adsorbents of accessible surface areas, large pore volumes, and narrow pore size distribution for the CO₂ capture. These studied solid adsorbents can provide an additional contribution and effort to develop an efficient CO₂ capture method as means of alleviating the serious global warning problem.