A critical review of the pulsed laser deposition (PLD) of amorphous diamond-like carbon (DLC) films is presented. A short review of the PLD process is followed by a review of various experimental configurations for DLC deposition and a discussion of the influence of process parameters on the composition and energy of ablated carbon plumes. Particular emphasis is given to the relationship between plume properties and film structure and mechanical characteristics. For the first time, a cumulative influence of the laser power density (fluence) and wavelength on the formation and properties of DLC films is shown. The influence of bias, additional auxiliary energy, substrate temperature, and the presence of hydrogen is also discussed. A fluence-wavelength region for DLC formation is proposed and correlated with the kinetic energy of ablated carbon species. It is shown that lower fluences are required to produce DLC films when shorter-wavelength lasers are used. The latest available results on applications of PLD DLC films as protective coatings for reducing friction and wear are also discussed. Methods are proposed to improve film adhesion to steel substrates, so that DLC films can be used in highly loaded friction contacts. Finally, process improvements that are necessary to permit scaling up PLD for growing DLC films are outlined.