Alpha case (an oxygen enriched alloy layer) is commonly formed in forged titanium alloys during the manufacturing process and it reduces the service life of the materials. This layer is normally removed mechanically or chemically. This paper reports the feasibility and characteristics of using a short pulsed laser to remove oxygen-enriched alpha case layer from a titanium alloy (Ti6Al4V) substrate. The material removal rate, i.e., ablation rate, and ablation threshold of the alpha case titanium were experimentally determined, and compared with those for the removal of bulk Ti6Al4V. Surface morphologies of laser processed alpha case titanium layer, especially that of cracks at different ablated depths, were carefully examined, and also compared with those for Ti6Al4V. It has been shown that in the alpha case layer, laser ablation has always resulted in crack formation while for laser ablation of alpha case free Ti6Al4V layers, cracking was not present. In addition, the surface is rougher within the alpha case layer and becomes smoother (Ra – 110 nm) once the substrate Ti-alloy is reached. The work has demonstrated that laser is a feasible processing tool for removing alpha case titanium, and could also be used for the rapid detection of the presence of alpha case titanium on Ti6Al4V surfaces in aerospace applications.