2,4-Dichlorophenol (2,4-DCP) is considered as an important pollutant because of its high toxicity and wide distribution in wastewaters. Innocuous remediation technologies have been studied for the removal of this pollutant. This study investigated the feasibility of using garlic roots as a plant system for the removal of 2,4-DCP. The optimal conditions for its removal were established based on orthogonal experiments (OA(25) matrix). Significant factors that affect removal efficiency, arranged from high to low importance, include pH, reaction time, 2,4-DCP concentration, and H2O2 concentration. In addition, garlic roots could be re-used for as much as three consecutive cycles. The decrease in pH and the increase of Cl- ion content in the post-removal solutions indicated that 2,4-DCP dehalogenation occurred during transformation. Changes in the deposition pattern of lignin in roots exposed to 2,4-DCP suggested that several of the products deposited were lignin-type polymers. The acute toxicity test revealed that the post-removal solutions were less toxic than the parent solutions. Therefore, garlic roots have considerable potential to effectively and safely remove 2,4-DCP from wastewater.