Social restriction in cities to curb infection rates of COVID-19 has become an opportunity to investigate the relationship between humans and the urban atmosphere. We evaluate the impact of the decline in human activities as a result of social distancing on the urban CO2 concentrations and air quality in Seoul during February and March of 2020 compared to 2019. Due to the reduction in human activity in 2020, local measurements of CO and NO2 show a decrease in background concentration (up to 11.9% and 41.7%, respectively) and urban enhancement (up to 16.7% and 38.1%, respectively) compared to the previous year. In contrast, the background concentration of CO2 increases by 3.9% in 2020. Ratios of CO:CO2 and NO2:CO2 also show a decrease in 2020 compared to the previous year, signaling an improvement in the urban air quality of Seoul. Moreover, the insignificant change in wind speed and wind direction during the months of February and March 2020 compared to 2019 implies that CO2, CO, and NO2 concentrations have not been influenced by meteorological conditions, but mainly by changes in emissions from decreased human activity. Despite the rise in background CO2 concentration, urban contributions of CO2 show a decline of 12.6%, indicating that cities with high emissions have the potential to reduce urban CO2 enhancements and air pollutant concentrations, and ultimately impact the global atmosphere.