The coupling of microscale zero-valent iron with autotrophic hydrogen bacteria (mZVI-AHB) are often believed to show greater potential than the single abiotic or biotic systems in remediating chlorinated aliphatic hydrocarbon-contaminated groundwater. However, our understanding of the remediation performance of this system under real field conditions, especially by incorporating the concept of sustainable remediation, remains limited. In this study, the performances of the mZVI, H2-AHB, and mZVI-AHB systems in dechlorinating groundwater containing complex electron acceptors were compared by evaluating their removal efficiency (RE), reaction products, and electron efficiency (EE), using trichloroethylene (TCE) as the target contaminant and NO3- and SO42- as the coexisting natural electron acceptors. Ultimately, which of these systems had TCE removal superiority was dependent on the coexisting electron acceptor. mZVI-AHB and mZVI resulted in more complete dechlorination, whereas H2-AHB exhibited higher N2 selectivity in reducing NO3-. Regardless of the coexisting electron acceptor, the mZVI-alone system showed the highest EE. Finally, the sustainability concerns and applicability of the three systems were evaluated on the basis of their TCE RE, complete dechlorination ratio, N2 selectivity, EE, and cost, which were integrated into a comparison of overall benefits. Our findings provide comprehensive and insightful information on the factors that determine remediation scheme selection in real practice.