Air pollution control has become the top priority of China’s “green development” concept since 2013. The Chinese government has enacted a range of policies and statutes to control contaminant emissions and improve air quality. On the basis of the national air quality ground observation database, the spatial and temporal distribution of air quality index value (AQI), fine particulate matter (PM_2.5), coarse particles (PM₁₀), sulfur dioxide (SO₂), nitrogen dioxide (NO₂), carbon monoxide (CO), and ozone (O₃) were explored in 336 cities throughout China from 2014 to 2019. AQI and most pollutants (except O₃) decreased in concentrations from 2014 to 2019. In 2019, all cities except Henan reached the level 2 of the ambient air quality index, and six cities had a lower ambient air quality index and reached the level 1. Spatially, higher pollutant concentrations were concentrated in large city clusters, whereas the areas with high O₃ concentration were found across the country. Furthermore, central heating was shown to have a negative impact on air quality. The observed AQI value, PM_2.5, PM₁₀, SO₂, NO₂, and CO concentrations were highest in north and northwest China and Henan province in central China. The correlations among pollutants suggest that the main sources of pollutants are fossil fuel combustion, industrial production, and motor vehicle emissions. The influence of meteorological factors on air quality, long-distance transportation, and the transformations of pollutants should be explored in future research.