Reductive dechlorination of chlorophenols by nickel coated iron was investigated to understand the feasibility of using Ni/Fe for the in situ remediation of contaminated groundwater. Zero valent iron (ZVI) was amended with Ni(II) ions to form bimetal (Ni/Fe). Dechlorination of 4-chlorophenol and formation of intermediates was studied using Ni/Fe. Effects of initial contaminant concentration, bimetal loading, presence of humic acid, and solution chemistry were also evaluated. Experimental results showed that Ni/Fe bimetal was so effective that more than 95% of 4-CP degradation was achieved within 240 minutes. Pseudo first-order rate constant for the dechlorination reaction was well correlated with bimetal loading. Humic acid competed for the reactive sites on the nickel coated iron with chlorophenols, lowering the dechlorination efficiency. No significant changes in solution pH were observed in the dechlorination of chlorophenols with Ni/Fe in the absence of buffer, indicating that reactivity of bimetal (Ni/Fe) could be prolonged. Phenol was found as a dechlorination intermediate of the conversion of 4-chlorophenol compound by Ni/Fe.