In this paper, plasma fluorination is combined with plasma silicon deposition to achieve step gradient modification on an epoxy resin surface. The physicochemical characteristics of samples are investigated and the electrical performances measured. The obtained results show that compared with untreated and single treated samples, the samples treated by step gradient modification significantly improve the flashover performance. According to experiment and simulation, the mechanism explanations are summarized as follows. First, it is found that the step gradient conductivity can effectively optimize the electric field distribution of a needle-needle electrode. Then, step gradient modification suppresses the accumulation of surface charge at the triple junction and makes the charge distribution more uniform. Furthermore, it can accelerate the surface dissipation on a high electrical field region and control the dissipation rate on a low electrical field region. All these results can restrain surface discharge and increase the flashover voltage. The step gradient modification method proposed in this paper provides a new idea for improving the surface insulation performance.