Owing to the strong ability to immobilize and hyperaccumulate some toxic heavy metals in contaminated soils, the biochar, lime and such as hyperaccumulator ramie received increasing interests from crops and environment safety in recent years. Outdoor pot experiment was conducted to compare the impacts of lime and biochar addition in paddy rice treatment, hyperaccumulator ramie and ramie combined with EDTA of plant Phytoremediation methods on soil available Cd dynamics in rainfall runoff and the mobility along soil profile, under both natural acid precipitation and acid soil conditions. The results showed that, biochar addition at a 2% mass ratio application amount significantly increased soil pH, while ramie with EDTA application obviously decreased soil pH compared to ramie monoculture. Within the same rainfall events, water soluble Cd concentration in surface runoff of ramie treatments was significantly higher than those of waterlogged rice treatments, and Cd concentration in runoff was obviously increased after EDTA addition, whereas lime at a 0.3% mass ratio application amount as additive had no obvious impact on soil pH and Cd speciation change, which may be due to the low application amount. During the whole experimental period , water soluble Cd concentration of rainfall runoff in spring was higher than that in summer, showing the same seasonal characteristics in all treatments. Biochar addition could significantly decrease available Cd content in 0-20 cm soil layer and with certain preferable persistency effects, whereas EDTA addition treatment obviously increased available Cd of 0-20 cm soil layer compared to other treatments, and obvious Cd element activation phenomenon in 20-40 cm soil layer was observed after EDTA addition. In conclusion, lime and biochar as environmental and friendly alkaline Cd immobilization materials showed lower environment risk to surface and ground receiving water, but attention should be paid to phytoremediation enhanced with EDTA or other organic acid before promotion and field application for heavy metals removal from contaminated soils.