Coordinated development of economy and environment is the common responsibility and pursuit of the international community. In this context, China is beginning to transform and upgrade its economy in a new model of coordinated economic and environmental development. Taking the VOCs emissions of atmospheric pollutants as object of study, this paper studies the relationship between environmental governance of pollutants emission and economic growth in Hunan Province, its characteristics, and also the mechanism of the relationship between the two. Besides, it also studies the measurement of the coordinated development of environment and economy. The study found that after 2015, the pollutant emission index of Hunan Province showed a linear downward trend, and the coordination degree between the environment and economic system decreased first and then gradually increased in the defined interval of coordination degree. The source of economic growth in Hunan Province comes from capital investment and environmental consumption. The improvement of environmental performance in Hunan Province is mainly driven by technological progress, and the emission reduction effect restricts the further growth of environmental performance.