Based on Gross Domestic Product (GDP) and 1km×1km land use data for 1980, 1990, 2000, and 2010, and using 2853 counties or districts as basic units, this study used models such as Ecosystem Service Value (ESV), Year of Economy-Environmental Harmonize (YEEH), and Economy-Environmental Harmonize Change(EEHC) and calculated the relationship between the economy and eco-environment according to the per unit area change of ESV and GDP. YEEH and EEHC indices were used to reflect the relationship between economic development and eco-environment systems of China and its evolution. The results showed that the coordination between economy and eco-environment continuously improved from 1980 to 2010. The EEHC in northern China was better than that in the western region, and the EEHC in western China was better than that in the central and eastern regions, reflecting the sustainable development of relationships between socio-economic activities and natural ecological environments. The spatial distribution of coordination between economy and eco-environment in China appeared aggregated model and its value was lower than the average in 1980. However, it developed to both high and low aggregation patterns in 2010. Furthermore, the degree of coordination between economic society and ecological environment changed for the better, but the distribution in different regions was very different and apparent. The results also showed that the economy should be developed when the ecological environment in the western region is protected, whereas ecological maintenance and restoration need to be considered when developing the economy in the central and eastern regions. There is still a long way to go for China's economic development and ecological environmental construction.