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The evaluation of urban sustainability plays a crucial role in the process of the sustainable development of cities. To decrease subjectivity and attain a comprehensive evaluation, this paper develops an evaluation method using the technique for order preference by similarity to ideal solution (TOPSIS). First, an evaluation index system including 39 indices and three categories (economic, social, and ecological development) is established; second, based on the index system, a modified TOPSIS, in which the entropy method is used to assign weights to each index according to its evaluation score and grey relation analysis is used to reduce the uncertainty existing in the process of evaluation, is presented to rank the sustainability level of cities. Finally, an example with the sustainability evaluation of 16 cities in the Anhui province of China is introduced to verify the effectiveness of the model.