Enhancing carbon fixation in the composting process was of great significance in the era of massive generation of organic solid waste. In this study, the experimental results showed that the contents of dissolved organic matter (DOM) in the experimental group (CT) were 37.58% higher than those in the control group (CK). The CO2 emission peaked on day 5, and the value of CK was 1.34 times that of CT. Significant differences were observed between the contents of sulfur fractions in CT and CK. This phenomenon may be due to the suppression of sulfur-reducing gene expression in CT. On day 51 of composting, the abundance of sulfur-oxidizing bacteria (SOB) Rhodobacter (5.33%), Rhodovulum (14.76%), and Thioclava (23.83%) in CT was higher than that in CK. In summary, the composting fermentation regulated by Fe2(SO4)3 increased the sulfate content, enhanced the expression of sulfur-oxidizing genes and SOB, and ultimately promoted carbon sequestration during composting.