Al-rich cubic (c-) Al
xTi
1−xN (
x ≈ 0.8) coating comprising self-organised c-Al(Ti)N/c-Ti(Al)N nanolamellae was prepared in a previous study by low-pressure chemical vapour deposition (LP-CVD) using an AlCl
3–TiCl
4–NH
3–Ar–H
2 precursor system. In the present study, we investigated the effects of isothermal annealing at 800 to 1200°C for 1 to 10 h on the crystal structure, microstructure, and hardness of the coating, and compared them to those of a monolithic c-Al
xTi
1−xN (
x ≈ 0.6) coatings prepared by arc-evaporated physical vapour deposition (PVD). The X-ray diffraction patterns indicated high phase stability of the former coating up to 1200°C after 1 h. High-resolution transmission electron microscopy revealed that the nanolamellae in c-Al
xTi
1−xN (
x ≈ 0.8) coating remained stable after post-annealing at 900°C for 5 h. The spontaneously formed coherent nanostructure suppressed diffusion in this coating, and the spinodal decomposition and hexagonal phase formation were thus shifted to higher temperatures. Consequently, age hardening in LP-CVD c-Al
xTi
1−xN (
x ≈ 0.8) helped to maintain its hardness at up to 1100°C after 10 h. The improved thermal stability and hardness at elevated temperature of the Al-rich c-Al
xTi
1−xN coating by LP-CVD led to a significant improvement in the cutting tool life, by factors of 2 and 10 compared to state-of-the-art CVD- and PVD-coated inserts, respectively. These improvements in thermal stability and elevated hardness in c-Al
xTi
1−xN (
x ≈ 0.8) coating prepared via LP-CVD process could remarkably enhance tool life for dry and high-speed cutting applications.
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