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Biological denitrification process in mainstream wastewater treatment often needs dosing supplemental electrons, consequently adding a remarkable operating cost. Organic carbon compounds are nowadays the most intensively used electron sources in full-scale wastewater treatment, corresponding with the well-understood carbon-nitrogen biogeochemistry for heterotrophic denitrification process. In the twenty-first century, the low-carbon technology is on calling to reduce the carbon footprint and relieve climate changing threatens. Autotrophic denitrification is highly recommended for mainstream wastewater treatment. The reduced-sulphur compounds (such as sulphide, elemental sulphur, and thiosulphate) could be utilised as electron donors, to drive sulphur cycle reactions to reduce nitrate and nitrite to dinitrogen gas. Based on the literature review and our own research experiences, this paper presents our perspectives on sulphur-driven autotrophic denitrification. It particularly focuses on the functional enzymes, sulphur bioreactors, and influential operating factors. Overall, this paper provides new insights on sulphur-nitrogen biogeochemistry and application as a low-carbon technology for nitrogen removal during municipal wastewater treatment.