Polymer–inorganic hybrid nanocomposites exhibit enhanced material properties, combining the advantages of both their organic and inorganic subcomponents. Extensive research is being carried out to functionalize polymers towards various improved physicochemical characteristics such as electrical, optical, and mechanical properties for various applications. Vapor-phase material infiltration is an emerging hybridization route, derived from atomic layer deposition, which facilitates uniform incorporation of inorganic entities into a polymer matrix, leading to novel applications in fields such as microelectronics, energy storage, smart coatings, and smart fabrics. In this article, recent advances in employing vapor-phase material infiltration as a hybridization and nanopatterning technique for various application avenues are reviewed.