Emerging laser precision machining, particularly using pulsed lasers, enlightens the innovation and functionalization of cemented carbides. These backbone materials of the tooling industry are usually considered difficult to machine or shape using conventional mechanical approaches. The coating of cemented carbide tools, deemed to improve their mechanical and thermal properties, is a common supplementary surface treatment prior to their application. This work aims to study the synergic effects of nanosecond laser ablation and coating deposition on the surface, as well as the mechanical integrity of cemented carbides. In this regard, two plain WC–Co grades with different metallic binder content (10%wtCo and 15%wtCo) were first processed by a short-pulsed nanosecond laser. Subsequently, an AlTiN film was physically vapor-deposited on the laser-processed surfaces. The resulting surface integrity was assessed in terms of topographical, morphological, and microstructural changes. Mechanical integrity was evaluated in terms of indentation and sliding contact responses using Vickers hardness and scratch tests, respectively, the latter including frictional, penetrating, and sliding performances under selected surface processing conditions. In general, the nanosecond laser ablation proved to be beneficial for the mechanical integrity of coated cemented carbides in most studied cases, as it increased surface hardness, reduced penetration depth, and hindered damage during sliding. This was the case despite a slight increase in surface roughness, as well as minor morphological and microstructural changes at the coating–substrate interface, discerned.