Massive stockpiles of uranium (U) mine tailings have resulted in soil contamination with U. Plants for soil remediation have low extraction efficiency of U. Chelating agents can mobilize U in soils and, hence, enhance phytoextraction of U from the soil. However, the rapid mobilization rate of soil U by chelating agents in a short period than plant uptake rate could increase the risk of groundwater contamination with soluble U leaching down the soil profile. This review summarizes recent progresses in synthesis and application of chelating agents for assisting phytoremediation of U-contaminated soils. In detail, the interactions between chelating agents and U ions are initially elucidated. Subsequently, the mechanisms of phytoextraction and effectiveness of different chelating agents for phytoremediation of U-contaminated soils are given. Moreover, the potential risks associated with chelating agents are discussed. Finally, the synthesis and application of slow-release chelating agents for slowing down metal mobilization in soils are presented. The application of slow-release chelating agents for enhancing phytoextraction of soil U is still scarce. Hence, we propose the preparation of slow-release biodegradable chelating agents, which can control the release speed of chelating agent into the soil in order to match the mobilization rate of soil U with plant uptake rate, while diminishing the risk of residual chelating agent leaching to groundwater.