The removal of carbon disulfide (CS2) from gas streams via FeCu/AC catalyst modified by non-thermal plasma (NTP) were investigated. In particular, effects of treatment conditions on the catalyst’s properties were studied. The properties change in the catalyst after NTP modification is measured by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and scanning electron microscope (SEM). The results showed relatively high capacities of FeCu/AC catalyst modified by NTP for removal of COS. The catalytic activity and sulfur capacity of material enhanced due to the extended oxygen functional groups on the surface of carbons. In addition, the surface area and micro-pore volume on NTP-modified catalysts played another important role in the process of CS2 removal.