Aramid fiber (AF)/epoxy composites are often used as mechanical and insulating materials for ultra-high voltage (UHV) gas-insulated switchgear (GIS) insulation pull rods. However, the product performance is believed to be restricted by the poor adhesion between AF and the resin matrix, affecting the operation reliability of GIS. In this work, a cascade process was applied to modify the AF surface to improve interfacial behavior. The AF was first treated with air dielectric barrier discharge (DBD) at atmospheric pressure to obtain a rough surface and then reacted with toluene-2,4-diisocyanate (TDI) to introduce polar functional groups onto the surface. The plasma discharge power and treatment time were investigated as major parameters, and the aging effect was studied. The modified AF was characterized by scanning electron microscope (SEM), Fourier transform infrared spectrometer (FTIR), x-ray photoelectron spectroscopy (XPS), atomic force microscope (AFM), and filament yarn tensile test. The interfacial behavior of the AF/epoxy composite was analyzed by interfacial shear strength (IFSS) test of micro-bond specimen and interlaminar shear strength (ILSS) test of Naval Ordnance Laboratory (NOL) rings. Experimental results showed that polar functional groups were introduced onto the AF surface. The IFSS and ILSS of AF/epoxy composite were increased by 32.8% and 20.2% at most, respectively, and the tensile strength of the AF was mostly preserved. Moreover, with the increase in plasma discharge power, the interfacial strength of the modified AF/epoxy interface increased firstly and then decreased. The AF modified by TDI retained a relatively good modification effect after aging for some time. This study presents a cascade process for the AF surface modification with simplicity, effectiveness, and resource-saving, which is suitable for industrial applications.