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The infrared (IR) gas sensing technique is excellent for CO 2 gas detection systems that require high accuracy and safety standard; however, there is a significant barrier to its application due to its high cost and difficulty in miniaturization. CO 2 sensors that are functional within near- or short-wavelength IR have the potential to reduce this barrier. In this work, a highly sensitive plasmonic material based on nanostructured covellite copper sulfide (CuS), which exhibits desired localized surface plasmon resonance for surface-enhanced IR absorption (SEIRA) throughout near- and mid-IR ranges, was investigated. We prepared CuS thin films facilely in an additive manner based on a spatial successive ionic layer adsorption and reaction process at room temperature. The resulting CuS thin film possesses a structure consisting of hexagonal nanoflakes, and demonstrates significant SEIRA for 100 ppm CO 2 with an enhancement factor of 10 4 .