Silica aerogels are unique nanostructured materials that possess many distinctive qualities, including extremely low densities and thermal conductivities, very high surface-area-to-volume ratios, and large strength-to-weight ratios. Aerogels, however, are very brittle, and are not readily shaped using traditional machining operations. Ultrafast laser processing may provide an alternative for precision shaping and machining of these materials. This paper discusses investigations of ultrafast laser machining of aerogels for material removal and micromachining. The advantages of ultrafast laser processing include a minimal thermal penetration region and low processing temperatures, precision removal of material, and good-quality feature definition. In this work, an amplified femtosecond Ti:sapphire laser system is used to investigate the breakdown threshold, material removal rate, and specific issues associated with laser processing of aerogels, as well as recommendations for further investigations for these unique materials.