Structural modifications of tetrahedral amorphous carbon (ta-C) films, caused by single-pulse laser irradiation, were investigated. Graphitization of the films, content and size of sp 2 carbon clusters were analyzed by means of Raman spectroscopy. It has been shown that pulse duration, as well as laser fluence and wavelength of irradiation, strongly influence the processes of graphitization and ablation of the ta-C films. In particular, heating of the films by the laser beam leads to formation of sp 2 carbon clusters and their enlargement up to the size of several nanometers. Material transformation to graphitized fraction is much more efficient in case of ns pulse duration. In case of fs pulse duration, such factors as multiphoton absorption and evaporation of over-heated material from the surface at high laser fluence, shorter time of irradiation, and heat transfer to the inner layers of the film lead to relatively weak graphitization characterized by the maximum size of the sp 2 carbon clusters of about 1 nm.