Laser-induced breakdown spectroscopy (LIBS) was successfully used in on-line control of selective removal of cobalt from tungsten carbide hardmetal by pulsed UV laser surface ablation. The dependence of LIBS on number of laser shots was investigated at different laser fluences. The optimal laser fluence of 2.5 J/cm(2) suited for selective removal of cobalt from surface layer of hardmetal was confirmed. The result sample was also subject to different post-examinations to evaluate the feasibility of the application of LIBS in this laser ablation process. It was demonstrated that, monitoring of the emission intensity of cobalt lines could be used as a control parameter for selective removal of cobalt from surface layer of hardmetal by pulsed UV laser. The on-line implementation of the spectroscopic technique LIBS to the surface-ablation process provided important information about the optimal-ablation parameters.