Conventionally, a soil nail is a piece of steel reinforcement installed inside a hole drilled into the slope and filled with cement paste (CP) grout. Chloride penetration is a major deterioration mechanism of conventional soil nails as the CP grout is easy to crack with an uncontrollable crack opening when the soil nail is subject to loading or ground movements. Engineered Cementitious Composites (ECC) are a class of fiber-reinforced material exhibiting excellent crack control even when loaded to several percent of strain, and therefore, ECCs have great potential to replace traditional CP grout in soil nails for achieving a long service life. In this study, the chloride ion transport characteristics and electrically accelerated corrosion process of steel rebar in ECC and CP grouts are systematically studied. The rapid chloride ion penetration test results showed a reduction of 76% and 58% passing charges in ECC with 0.15% and 0.3% pre-loading strain, respectively, as compared to that in un-cracked CP. Furthermore, the accelerated corrosion experimental data showed that ECC under pre-loading strain still exhibited a coefficient of chloride ion diffusion that is 20–50% lower than CP grout due to the ability to control crack width. Service life calculations based on experimentally measured parameters showed that the predicted corrosion rate and corrosion depth of soil nails in ECC grout were much lower than those in CP grout. The findings can facilitate the design of soil nails with excellent durability and long service life.