In the present work, a low-pressure chemical vapor deposition (LPCVD) Ti0.17Al0.83N and state-of-the-art arc ion plating PVD-Ti1−xAlxN (x = 0.25, 0.55, 0.60, 0.67) coatings were deposited on cemented carbide substrate. The morphological, structural, and electrochemical properties of LPCVD-Ti0.17Al0.83N and PVD-Ti1−xAlxN coatings were compared. The X-ray diffraction (XRD) results and scanning electron microscopy (SEM) images revealed that the LPCVD-Ti0.17Al0.83N coating had a face-centered cubic (fcc) structure, while presenting a crack-free surface morphology and a compressive residual stress of −131.9 MPa. The PVD coatings with a composition of x ≤ 0.60 had an fcc structure, while the PVD-Ti0.33Al0.67N coating consisted of fcc and w-AlN phases. The results of the electrochemical corrosion test showed that the LPCVD-Ti0.17Al0.83N coating had the lowest corrosion current density in a 3.5 wt.% NaCl solution. After a 20-day immersion corrosion test in a 5 mol/L HCl solution, the LPCVD-Ti0.17Al0.83N coating displayed higher stability than the PVD-Ti1−xAlxN coating. The results of electrochemical impedance spectroscopy (EIS) and X-ray photoelectron spectroscopy (XPS) analysis revealed that more uniform and denser passivation film, as well as higher Al2O3 proportion in the Al2O3/TiO2 composite passive layer, led to the outstanding corrosion resistance of the LPCVD-Ti0.17Al0.83N coating.