Ultralow refractive index materials (n less than 1.38 at 550 nm) are of particular interest in the context of antireflective coatings, allowing one to enhance their overall optical performance. However, application of such materials is typically limited by their mechanical properties. In this study, we explore the characteristics of a new category of hybrid (organic/inorganic) SiOCH thin films prepared by glancing angle deposition (GLAD) using electron beam evaporation of SiO2 in the presence of an organosilicon precursor. The resulting layers exhibited n as low as 1.2, showed high elastic rebound, and generally better mechanical properties than their inorganic counterparts. In addition, hybrid GLAD films were found to be highly hydrophobic. The performance of the films is discussed in terms of their hybridicity (organic/inorganic) ratio determined by infrared spectroscopic ellipsometry as well as the presence of anisotropy assessed by the nanostructure-based spectroscopic ellipsometry model. Finally, we demonstrate successful implementation of the ultralow-index material in a complete antireflective stack.