The use of biodegradable chelating agents and fertilizer to improve phytoremediation is a cost-effective and environmental-friendly method for remediation of copper (Cu)- and cadmium (Cd)-polluted agricultural soil. A pot experiment was conducted to investigate the effects of phosphorus (P) fertilizer and the chelator ethylenediamine disuccinic acid (EDDS), both individually and in combination, on the phytoremediation efficiency of castor plants. The experiment included six treatments with three replicates, which were as follows: control (no P or EDDS), EDDS alone, P at 100 mg kg−1, P at 300 mg kg−1, P at 100 mg kg−1 + EDDS, and P at 300 mg kg−1 + EDDS. The results demonstrated that phosphorus significantly promoted the growth of castor plants. In the treatment in which 300 mg kg−1 P2O5 and 5.0 mmol kg−1 EDDS were added, the shoot dry weight and root dry weight increased by 42.0% and 67.6%, respectively, when compared to the treatment only applying EDDS, and this treatment significantly promoted the absorption of Cd by shoots of castor. In the absence of phosphorus application, EDDS significantly diminished the dry weight of castor roots by 27.3%. Nevertheless, it improved the concentrations of Cu in the shoots and roots of castor plants, which were 3.43 times and 3.27 times higher than those of the control, respectively. Furthermore, when combined with phosphorus fertilizers, EDDS further promoted the absorption of Cu and Cd in the shoots of castor, which significantly increased by 13.34 times and 0.47 times, respectively, with addition of 100 mg kg−1 phosphorus and 5.0 mmol kg−1 of EDDS compared with the control. Phosphorus and EDDS synergistically decreased the activity of POD enzymes in leaves and roots compared with those treated with only EDDS and alleviated the toxicity of EDDS and heavy metals to castor plants. These findings provide scientific evidence for the use of agronomic measures and chelators to optimize phytoremediation efficiency in Cu and Cd co-contaminated soils.