To overcome climate challenges, emerging CO2 capture technologies focus on innovative solid and chemical adsorbents like aerogels. Aerogels, in particular silica aerogel, have emerged as an exceptional class of materials with unique properties. In particular, functionalizing the silica matrix with metal oxides can significantly enhance their adsorption capacity and selectivity. For this reason, in this research, alumina is added to the aerogels to improve both mechanical and adsorption properties (due to the basic character of alumina). Furthermore, functionalizing alumina-silica aerogels with amino groups could improve their ability to adsorb CO2. Alumina-silica aerogels functionalised with amino groups (AlSi with (3-aminopropyl) trimetossisilano, also called APTES) for CO2 capture are here synthesized for the first time by a one-pot process.