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Carbon cycle regulation and greenhouse gas (GHG) emission abatement within wastewater treatment plants (WWTPs) can theoretically improve sustainability. Currently, however, large amounts of external carbon sources used for deep nitrogen removal and waste sludge disposal aggravate the carbon footprint of most WWTPs. In this pilot-scale study, considerable carbon was preliminarily recovered from primary sludge (PS) through short-term (five days) acidogenic fermentation and subsequently utilized on-site for denitrification in a wool processing industrial WWTP. The recovered sludge-derived carbon sources were excellent electron donors that could be used as additional carbon supplements for commercial glucose to enhance denitrification. Additionally, improvements in carbon and nitrogen flow further contributed to GHG emission abatement. Overall, a 9.1% reduction in sludge volatile solids was achieved from carbon recovery, which offset 57.4% of external carbon sources, and the indirect GHG emissions of the target industrial WWTP were reduced by 8.05%. This study demonstrates that optimizing the allocation of carbon mass flow within a WWTP has numerous benefits.