Excessive human activities destroy the structure and function of ecosystem and threaten sustainable development. As a typical resource-based area, Shanxi Province is facing an increasingly serious contradiction between ecosystem and sustainable development, with the overexploitation of resources. In view of this, the coupling coordination degree model was used to measure the association between sustainable development and ecosystem services (SDESs), and geographically and temporally weighted regression model was used to explore the correlation between SDESs and measure the correlation between ecosystem services (ESs) and sustainable development at the county level from 2000 to 2015 in Shanxi Province. The results showed an increase in the sustainable development level and all ESs except soil retention. The coupling coordination degree (CCD) of soil retention and sustainable development decreased, while other services increased. Habitat quality had the strongest negative correlation with sustainable development. There were obvious spatiotemporal heterogeneities in the CCD and correlation of SDESs, which is helpful for promoting regional sustainable development and optimize ecosystem decision-making.