Methods of making hydrophobic aerogels are described. Disclosed methods include forming a surface-modified metal oxide aerogel precursor from a sol comprising a solvent, a metal oxide precursor, and a hydrophobic surface modifying agent. The resulting modified precursor can be dried to from hydrophobic aerogels. Methods of forming the surface-modified metal oxide aerogel precursor include hydrolyzing the metal oxide precursor and co-condensing the hydrolyzed metal oxide precursor and the hydrophobic surface modifying agent. Hydrophobic aerogels and hydrophobic aerogel articles are also disclosed.
