Direct air capture (DAC) has been identified as a necessary negative emission technology (NET) to solve global warming. DAC methods have been divided into two major types: solvent absorption and sorbent adsorption. Aqueous amine absorption is the major method in postcombustion carbon capture, not in DAC because contactors blow large volumes of air over the solvent, which results in high evaporation of solvents. Solid amine adsorption has been one of the primary methods of DAC due to its low volatility of amine. Therefore, the development of DAC adsorbents is the key to improve CO2 capture efficiency. Nowadays, the research on adsorbents mainly focuses on amine impregnation and grafting. The grafting adsorbents generally have better stability than impregnation adsorbents. Silica is the most common support material for amine-grafted adsorbents. Nonetheless, silica has some defects, such as poor hydrothermal stability, which limits its employment. Alumina is a promising support material with excellent hydrothermal stability, but studies on amine-grafted alumina are still scarce. Herein, a method of 3-[2-(2-aminoethylamino)ethylamino] propyltrimethoxysilane (TRI) grafting onto γ-alumina is presented. The results of this paper suggest that alumina is a potential support material for amine grafting. The CO2 adsorption capacity of the adsorbent is 0.39 mmol g-1 at 400 ppm and 25 °C. The amine-grafted alumina has excellent thermal stability than the amine-impregnation silica adsorbent. Besides, the adsorbent exhibits stable performance during cycles, with the working capacity maintained at 83% of that of the first cycle after 60 cycles. Water adsorption capacity and selectivity indicate that TRI-Al2O3 has good selectivity at high relative humidity. These findings make amine-grafted alumina a promising DAC adsorbent.