As the contradiction between ecological protection and socioeconomic development continues to intensify, the balanced development of economy, resources, environment, and society has become a core issue in promoting the achievement of high-quality development. In this study, we proposed a framework for assessing China's ecological and economic security, from the perspective of national sustainable development. We also assessed the level and dynamic evolution pattern of the ecological and economic security of different provinces and regions, in terms of the dynamic characteristics of sustainable development. The results indicated that from 2005 to 2019, China's ecosystem sustainability level did not improve significantly, with prominent regional differences; notably, the country would need to deplete its natural capital stock for economic development. As of 2019, China achieved comprehensive and stable high-quality socioeconomic development, but there was a wide gap in the eco-economic efficiency of individual provinces. Currently, the efficiency of the use of natural capital needs improvement. In terms of the ecological and economic security of China's provinces, only the coastal economic zone maintained a safe level of ecological economy, while the rest of the provinces portrayed fluctuations. The convergent evolution of the state revealed that the ecological and economic security portrayed an overall upward trend. However, after considering the neighborhood effect, the ecological and economic security of the northern and southern regions increased, whereas that of the central and coastal regions decreased. This study can serve as a viable framework, to promote sustainable development in not just China, but also other global economies.