Municipal solid waste incinerator (MSWI) fly ash was used for accelerated carbonation via bubbling of gaseous carbon dioxide (CO2) after treatment with sodium hydroxide (NaOH). The influence of alkaline concentration and volumetric flowrate of CO2 was investigated. Experimental results showed that carbonation reduced the leaching of Cu, Pb, Zn, and Cr. The pH of leachate decreased from around 12 to 10.5. The content of soluble chlorides was also decreased after carbonation. Additionally, the application of accelerated carbonation enhanced the sequestration of CO2 from MSW incineration plants. The TG/DSC analysis indicated that MSWI fly ash sequestrated approximately 185 g CO2/kg waste.