TiAlN-based coatings are widely used in dry cutting due to their high hardness and thermal stability; however, their inherently high friction coefficient often leads to excessive thermal wear. To overcome this limitation, we developed a multilayer DLC/Cr/TiAlN composite coatings using physical vapor deposition (PVD), combining a hard TiAlN base layer, a ductile Cr interlayer for improved toughness, and a low-friction diamond-like carbon (DLC) top layer. To overcome the typically poor adhesion of PVD coatings, laser processing was conducted on the TiAlN coatings surface using air, deionized water, and Al₂O₃ nanofluid-assisted methods. The surface morphology, hardness, adhesion strength, and tribological performance were systematically evaluated. Results showed that Al₂O₃ nanofluid-assisted laser processing created defect-free textures, significantly enhancing mechanical properties: the TiAlN coating achieved a peak hardness of 30.382 GPa and a maximum adhesion strength of 3.65 N. The DLC/Cr/TiAlN composite coating exhibited a maximum adhesion strength of 2.03 N, with minimal friction coefficient during dry sliding, without evidence of delamination or ploughing. These findings demonstrate the efficacy of Al₂O₃ nanofluid-assisted laser processing in significantly improving the performance of DLC/Cr/TiAlN composite coatings for demanding dry friction application conditions.