This study fabricated AlCrSiN coatings from six alloy targets (Four Al7Cr3 targets and two Cr9Si1 targets) using high-power impulse magnetron sputtering (HiPIMS) with a focus on the effects of substrate bias voltage (−30 to −90 V) on deposition rate, microstructure, crystal orientation, residual stress, and mechanical properties. Electron Probe Microanalysis (EPMA) and X-ray Diffraction (XRD) results revealed that variations in bias voltage had little impact on the element composition or crystal structure (FCC) of AlCrSiN coatings; however, under high bias voltage (exceeding −60 V), the preferred orientation shifted from the (111) plane to the (220). Increasing the bias voltage from −30 to −90 V was shown to reduce the deposition rate (from 42.2 to 37.6 nm/min) and the thickness of the AlCrSiN coating (from 2.9 to 2.6 μm). It was also shown to increase the hardness (from 2147 to 3658 HV) and residual stress (from −0.01 to −0.59 GPa) by reducing the grain size and allowing the formation of a denser structure. Various interlayer designs (AlCr/AlCrxNy/AlCrN, CrSi/AlCrxNy/AlCrN, AlCr/CrSixNy/CrSiN, CrSi/CrSixNy/CrSiN) were assessed in terms of adhesion strength between the AlCrSiN and substrate. Under the same AlCrSiN deposition condition, with the bias voltage set to −60 V, the highest adhesion strength (from 32.28 to 45.81 N) was achieved using a CrSi/CrSixNy/CrSiN interlayer structure.