Climate warming and responses become the focus of international attention and academic research. Quantitative assessment of forest vegetation carbon sequestration is an important aspect of climate change research. Chizhou is the first eco-economy demonstration area in China and also the pilot city of construction in ecological Anhui Province. With forest inventory data from 2009, we used investigation, models, literature search and other methods to show carbon storage of forest vegetation in Chizhou based on calculating biomass of different stands and volume regression equations on the whole dry biomass. The total biomass of Chizhou is 35.988 790 million t; the total whole dry biomass 35.131 031 million t; the total carbon storage is 17.161 3 million t, and the carbon density is 34.70 t·hm^–2. This article can help government departments and increase public awareness about the huge forest vegetation ecosystem services of carbon sequestration in Chizhou to provide a theoretical basis for establishing the eco-city development strategy; it also enhances the enthusiasm and initiative of forest vegetation protection in Chizhou.