In order to further improve the insulation performance of fiber reinforce plastic (FRP) materials used in electromagnetic pulse (EMP) simulators, the flashover characteristics of FRP materials with different surface roughness and groove, i.e., those who are easily achieved and have a prominent effect, are investigated in 0.1 MPa SF6 under nanosecond pulse voltage with a rise time of 20–30 ns. The experimental results show that surfaces with different roughness have no significant influence on the flashover voltages of the FRP insulators, and both the convex grooves made of FRP and the convex grooves with nylon rings inlaid to form projections can improve the surface flashover voltage of epoxy FRP insulators under nanosecond pulse, in which the effect of the former surface is more obvious. For the insulators with convex grooves made of FRP, it is found that the root of the FRP protrusions breaks down after a number of shots with the occurrence of carbonization channels and spots, which is nonexistent for the nylon projections. Combined with the test results of surface characteristics, the surface roughness and the secondary electron emission yield (SEEY) are not key factors of flashover characteristics in SF6 under nanosecond pulse, arguably due to the fact that the energy needed for an incident electron to ionize an SF6 molecule is lower than that to excite two secondary electrons. Hence, the flashover performance cannot be improved by adjusting the surface roughness, and the flashover channel is principally governed by the macroscopic distribution of electrical field which can be changed by the convex groove. Breakdown phenomena of FRP protrusions indicate that the bulk insulation performance of resin FRP is weaker compared to pure resin because of its composite structure, as well as the impurities and voids introduced in the manufacturing process. The results are instructive for the design of FRP insulation structures in the compact EMP simulator.