The methods of ecological footprint and decoupling effect analysis are effective tools for measuring the status of sustainable development in a region. Taking Hefei as an example of rapid development of urbanization, this article applied the analysis of an ecological footprint and decoupling effect to conduct the quantitative research and dynamic analysis of the ecological status from 2000 to 2014. Additionally, the GM (1, 1) model was established to predict the ecological status of Hefei from 2015 to 2020. The results show that from 2000 to 2014, the per capita ecological footprint of Hefei and the per capita ecological carrying capacity fluctuated. The fluctuation of the ecological deficit was small and increased slightly in general. The ecological footprint of fossil fuels was relatively large in recent years. The space distribution of the ecological footprint and carrying capacity is low in the urban district and high in the suburban district. In the decoupling relationship between environmental pressure and economic growth, the frequencies of strong decoupling and weak decoupling were 42.9% and 28.6%, respectively. The grey model predicts that the per capita ecological footprint from 2015 to 2020 will also increase. This finding is significant for optimizing the industrial structure of Hefei City, implementing different land use patterns, upgrading land patterns, and for controlling population growth moderately.