Nanosecond-pulsed Nd:YAG laser ablation was investigated as a method for removing Al Ti-based hard coatings deposited on WC–Co hardmetal inserts. Systematic variation in laser parameters identified conditions for complete coating removal while preserving substrate integrity. The laser was operated at 532 nm, under a range of fluences (0.1–11.7 J/cm²), pulse delays (20–180 µs), and pulse numbers (1–300). LIBS qualitative monitoring enabled precise ablation progress by identifying Ti, Al, and O layers, and later the detection of Co and W signals. Scanning electron microscopy (SEM/EDS) and optical profilometry confirmed that 5–10 pulses at intermediate delays (60–80 µs, 4.8–7.1 J/cm²) provided complete removal of ~18 µm-thick coatings while maintaining substrate integrity. In contrast, higher energies and excessive pulses caused localized melting and surface irregularities. These results demonstrate that Nd:YAG laser ablation, especially when coupled with LIBS, offers a precise, fast, and environmentally alternative to conventional chemical stripping methods for the refurbishment and recycling of cutting tools.