Metal sulfide-based biological process is considered as a promising biotechnology for next-generation wastewater treatment. However, it is not clear if simultaneous bio-reduction of nitrate and chromate was achievable in this process. This study aimed to evaluate the feasibility of metal sulfides (FeS and MnS) on simultaneous denitrification and chromate reduction in autotrophic denitrifying column bioreactors. Results showed that simultaneous reduction of nitrate and chromate was achieved using metal sulfides (FeS and MnS) as electron donors, in which sulfate was the sole soluble end-product. Apart from the sulfur element in the metal sulfides, Fe(II) and Mn(II) were also involved in nitrate and chromate reduction as indicative by the formation of their oxidative states compounds. In microbial communities, SHD-231 and Thiobacillus were the most predominant bacteria, which might have played important roles in simultaneous denitrification and chromate reduction. Compared to FeS, MnS showed a higher performance on nitrate and chromate removal, which could also reduce the toxic inhibition of chromate on nitrate reduction. According to results of XRD and XPS, as well as a lower sulfate production in the FeS system, FeS might have been covered easily to hydroxides due to its bio-oxidation, which limited mass transfer efficiency and bio-availability of FeS. The findings in this study offered insights in the development of promising approaches for the treatment of toxic and hazardous compounds using metal sulfide.