This paper reviews thin films constituted by elements based on the Ti-Al-N system, bearing in mind the role of the condensed phases in the development of structural components and functional devices. In recent decades, the Ti-Al, Ti-N and Al-N nanocrystalline binary systems have rapidly attracted research and industry interest. These systems have revealed a great performance via atomic-level structural control, making it possible to tailor new atomic structures and morphologies suitable in different applications as protective and hard coatings and as thermal/diffusion barriers. The binary phases based on nitrogen were the first to exhibit a wealth of interesting mechanical and electrochemical behaviours. However, more recently the Ti-Al and, particularly, the Ti1 -x Al (x) N thin films have been applied with success in the industry. The purpose of this paper is to compile the master results concerning the production and characterisation of binary and ternary thin films of the Ti-Al-N system using similar deposition strategies. These materials form a good base to analyse the correlation between the chemical composition and the atomic structure, the preferred orientations and the morphology of 2D monolithic materials. The deposition strategies adopted and the thin films' chemical compositions determine the as-deposited structures and, consequently, the mechanical behaviour of the thin films produced, particularly the hardness. In general, an intermediary amorphous stage is observed, i.e., the thin films exhibit a loss of crystallinity in the transition from a saturated solid solution to a new compound.