In the present work, the effect of implantation sequence on tribological behavior of GCr15 steel treated by plasma-based ion implantation of carbon and nitrogen has been investigated. The treated GCr15 steels were characterized for microstructure and abrasive wear performance through combination of Raman spectroscopy, nano-indentation, and wear tests. Raman spectroscopy indicated that diamond-like carbon (DLC) films were formed after implantation of carbon with or without implantation of nitrogen, and the implantation of nitrogen after the implantation of carbon destroyed the graphite structure of the DLC films. The nano-indentation and wear tests showed that nanohardness as well as wear resistance of the GCr15 steel treated with the implantation sequence of nitrogen-carbon was better than those with the implantation sequence of carbon-nitrogen. Meanwhile, the properties were improved with increasing of carbon ion fluence.