Adaptive nanocomposite coating materials that automatically and reversibly adjust their surface composition and morphology via multiple mechanisms are a promising development for the reduction of friction and wear over broad ranges of ambient conditions encountered in aerospace applications, such as cycling of temperature and atmospheric composition. Materials selection for these composites is based on extensive study of interactions occurring between solid lubricants and their surroundings, especially with novel in situ surface characterization techniques used to identify adaptive behavior on size scales ranging from 10−10 to 10−4 m. Recent insights on operative solid-lubricant mechanisms and their dependency upon the ambient environment are reviewed as a basis for a discussion of the state of the art in solid-lubricant materials.