Abstract: Geological storage of CO2 has become one of the effective ways for reducing greenhouse gas emissions. Regional suitability evaluation of geological storage of CO2 is the basis of choosing sites of construction of geological storage of CO2. Establishment of proper evaluation index systems and selection of reasonable evaluation methods play a crucial role in the suitability evaluation of geological storage of CO2. For the propose of CO2 reduction needs of Anhui Province, according to the actual geological conditions of the study areas and from the multiple aspects of associated CO2 geological storage, the research built an evaluation index system of four aspects, which include security, technicality, economy and social environment. The variation coefficient method is introduced to determine the weight and the TOPSIS model is used for ranking the suitability of CO2 geological storage basin in the study areas. The results of the evaluation show that the Fuyang Basin and the Hefei Basin are prior selection for geological storage of CO2. The evaluation results provide a scientific evidence for preliminary choosing engineering construction of geological storage of CO2.