BackgroundRecently, we have developed a new soil electrokinetic remediation (SEKR) process, hereinafter referred to as the perforated cathode pipe SEKR system (PCPSS), to achieve remediation intensification. Some obstacles, such as the low removal of some heavy metals, particularly Ni, limited our previous PCPCS. MethodsWe aim to improve the removal efficiency of the PCPSS by adding a chelating agent (i.e., ethylenediaminetetraacetic acid (EDTA)). Given the unsatisfactory remediation results obtained in our previous studies, the Taguchi approach (L9OA) was exploited in this work as an experimental design to determine the optimal level of factors that could enhance Ni removal. Significant findingsResults showed that an electric potential of 3 V, addition of 0.5 mol of EDTA, and an initial Ni concentration in the range of 10–20 mg kg−1 could optimize Ni removal. Confirmation experiments conducted on natural contaminated soil showed the following order of removal of heavy metals and other elements: Al (70%) > Co (69%) > Fe (63.5%) > Cu (55%) > Mn (52.8%) > Zn (43.17%) > Cr (41.41%) > Ni (22.26%). Among the studied soil cations, Mg showed the best removal rate, Ba showed moderate removal rate, and Ca showed the lowest removal rate. Notably, the removal rate of V was much higher than that of born (B).