A new approach was adopted to integrate the promising performances of TiAlN and TiCN ternary films for applications in extreme environments. In this study, Al,C-co-doped δ-TiN films, that is, TiAlCN quaternary films, were fabricated using a novel multi-arc ion plating and direct current (DC) magnetron sputtering (MIP&DCMS) integrated technique. The sandwich-like gradient architecture of the TiAlCN quaternary films altered the columnar crystal nature of the δ-TiN matrix and yielded fine grains, finally producing a heterophase composite structure. This structure contributed to its high microhardness (36.8 ± 1.6 GPa) and elastic modulus (410 ± 22 GPa) while maintaining superior tribological characteristics, with a friction coefficient of 0.26 ± 0.03. The TiAlCN quaternary films provided excellent corrosion resistance to SS304 with a corrosion current density of 0.129 ± 0.116 μA cm−2 and a polarization resistance of 430.5 ± 10.56 kΩ cm2, which are comparable to those of emerging TiAlN and TiCN ternary films.