In recent years, as China’s peaking carbon dioxide emissions and air pollution control projects have converged, scholars have begun to focus on the synergistic mechanisms of greenhouse gas and pollution gas reduction. In 2020, the unprecedented coronavirus pandemic, which led to severe nationwide blockade measures, unexpectedly provided a valuable opportunity to study the synergistic reduction in greenhouse gases and polluting gases. This paper uses a combination of NO2, O3, and CO2 column concentration products from different satellites and surface concentrations from ground-based stations to investigate potential correlations between these monitoring indicators in four Chinese representative cities. We found that XCO2 decreased in March to varying degrees in different cities. It was witnessed that the largest decrease in CO2, −1.12 ppm, occurred in Wuhan, i.e., the first epicenter of COVID-19. We also analyzed the effects of NO2 and O3 concentrations on changes in XCO2. First, in 2020, we used a top-down approach to obtain the conclusion that the change amplitude of NO2 concentration in Beijing, Shanghai, Guangzhou, and Wuhan were −24%, −18%, −4%, and −39%, respectively. Furthermore, the O3 concentration increments were 5%, 14%, 12%, and 14%. Second, we used a bottom-up approach to obtain the conclusion that the monthly averaged NO2 concentrations in Beijing, Shanghai, and Wuhan in March had the largest changes, changing to −39%, −40%, and −61%, respectively. The corresponding amounts of changes in monthly averaged O3 concentrations were −14%, −2%, and 9%. However, the largest amount of change in monthly averaged NO2 concentration in Guangzhou was found in December 2020, with a value of −40%. The change in O3 concentration was −12% in December. Finally, we analyzed the relationship of NO2 and O3 concentrations with XCO2. Moreover, the results show that the effect of NO2 concentration on XCO2 is positively correlated from the point of the satellite (R = 0.4912) and the point of the ground monitoring stations (R = 0.3928). Surprisingly, we found a positive (in satellite observations and R = 0.2391) and negative correlation (in ground monitoring stations and R = 0.3333) between XCO2 and the O3 concentrations. During the epidemic period, some scholars based on model analysis found that Wuhan’s carbon emissions decreased by 16.2% on average. Combined with satellite data, we estimate that Wuhan’s XCO2 fell by about 1.12 ppm in February. At last, the government should consider reducing XCO2 and NO2 concentration at the same time to make a synergistic reduction.