In the present work, aluminosilicate aerogels prepared under various conditions were compared with respect to their nanostructures and porosity. The purpose of this investigation was to find a suitable way to predict the final product structure and to tailor a required texture. Several Al and Si precursors (Al nitrate, Al isopropoxide, Al acetate, tetraethoxysilane (TEOS), and sodium silicate) were used in our examinations; the solvent content (water and alcohols), surfactants, as well as the catalysts were varied. In addition, the aerogels were subjected to various heat treatments. Hybrid aerogels were synthesized by the addition of different polymers (poly(acrylic acid), polyvinyl acetate, and polydimethylsiloxane). Aluminosilicate and hybrid aerogel structures were investigated by 27Al MAS NMR, SAXS, SEM, and porosity measurements. Loose fractal structures with a good porosity and high Al incorporation can be achieved from TEOS and Al nitrate or isopropoxide via a sol-gel preparation route. The use of Al acetate led to compact aerogel structures independently of the Si precursor, the pH, and the catalyst.