In this study, we applied an emerging, environmentally friendly surface engineering technology, electrolytic plasma processing (EPP), for the surface modification of Q195 structure carbon steel surface pretreatment and further Zn coating. Treating the surfaces of Q195 structure carbon steel by EPP was a quite dynamic process, which was investigated using scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), and X-ray diffraction (XRD). The results shown that surface scale can be effectively remove after 40 s EPP treatment, and the EPP-treated Q195 structure carbon steel revealed a slight decrease in elastic modulus and hardness, but a substantial improvement in tensile (especially plastic) mechanical properties. Moreover, the further EPP modification conducted on the pretreated Q195 structure carbon steel sample for production of a layer of compact zinc coating with 15 μm thickness under an optimization EPP process. We also identified the modification mechanism of EPP to Q195 structure carbon steel, which may provide theoretical and practical guidance for future researchers and developers.