Polycarbonate (PC) and protective (Ti,Al)N coatings exhibit extremely different material properties, specifically crystal structure, thermal stability, and elastic and plastic behavior, as well as thermal expansion coefficients. These differences present formidable challenges for the deposition process development as low-temperature synthesis routes have to be explored to avoid a thermal overload of the polymer substrate. Here, a large-area sputtering process is developed to address the challenges by systematically adjusting target peak power density and duty cycle. Adhering (Ti,Al)N coatings with a critical residual tensile stress of 2.2 ± 0.2 GPa are obtained in the pulsed direct current magnetron sputtering range, whereas depositions at higher target peak power densities, realized by high power pulsed magnetron sputtering, lead to stress-induced adhesive and/or cohesive failure. The stress-optimized (Ti,Al)N coatings deposited onto PC with a target peak power density of 0.036 kW cm−2 and a duty cycle of 5.3% were investigated by the cross-cut test, confirming adhesion. By investigating the bond formation at the PC|(Ti,Al)N interface, mostly interfacial CNx bonds and a small fraction of (C−O)−(Ti,Al) bonds are identified by x-ray photoelectron spectroscopy, indicating reactions at the hydrocarbon and the carbonate groups during deposition. Nanoindentation reveals an elastic modulus of 296 ± 18 GPa for the (Ti,Al)N coating, while a Ti–Al–O layer is formed during electrochemical impedance spectroscopy in a borate buffer solution, indicating protective passivation. This work demonstrates that the challenge posed by the extremely different material properties at the interface of soft polymer substrates and hard coatings can be addressed by the systematical variation in the pulsing parameters to reduce the residual film stress.