A review of a recent progress in developing new tribological materials for operating across multiple environments relevant to aerospace applications is provided. New coating materials were designed to rearrange their structure and chemistry on demand to adapt to variable surface conditions (environment humidity, temperature). These materials have been dubbed chameleon because of their ability to change their surface chemistry and structure to avoid wear. The chameleon coating concept involves a nanocrystalline/amorphous nanocomposite structure, where individual phases are arranged to provide a high degree of mechanical and thermal stability and, at the same time, serve as nano reservoirs for tribological surface self-reconstruction. The stored materials are released from nanophase reservoirs in the process of wear and tribological surface chemistry and structure change to continuously reduce friction and wear. This surface response is triggered by changes in the operating environment and/or temperature. Several mechanisms are employed, including self-induced crystallization of amorphous dichalogenide phases, nucleation of nanograins of low melting point metals, formation of low melting point glassy ceramics, and change in the electron hybridization of carbon. These mechanisms were explored in sliding wear tests performed in controlled humidity air, dry nitrogen, and vacuum, as well as at high temperature in air.