In this study, we developed composite Fe-Cr-V-C coatings by plasma transferred-arc (PTA) powder surfacing on a 42CrMo steel substrate. The effects of arc current and ion gas flow rate on the coatings’ microstructure, hardness, and bonding performance were investigated. During the surfacing process, VxCy,M7C3M=Fe,Cr and other hard phases are in-situ generated throughout the entire PTA powder surfacing. These phases are uniformly distributed in the Fe matrix through precipitation and dispersion strengthening, yielding a surface hardness of up to 64.1 HRC. Also, the bonding performance between the substrate and coatings was evaluated by measuring the tensile strength, revealing that strong metallurgical bonds are formed, reaching a strength greater than 811 MPa.