Anthropogenic emissions affect vegetation photosynthesis and carbon flux through meteorological variations induced by aerosols and clouds. However, the insufficient consideration of meteorological conditions limits the understanding of relevant mechanisms, and further inhibits the projection of future terrestrial carbon balance. Based on multiple sets of model simulations, we characterized changes in gross primary production (GPP) due to three typical individual pollutants emissions (black carbon, organic carbon, and sulfate), quantified the relative contributions of co-varied environmental factors, and explored the regulatory roles of background meteorological conditions across China. Our results showed that the heterogeneous GPP enhancement induced by emissions was dominated by cloud cover (CC) change. During its short-term effect, air temperature (Tair), vapor pressure deficit (VPD), and radiation (both quality and quantity) played a collectively non-negligible role in GPP variation, among which the universal diffuse radiation fertilization effect was generally far less than the benefits of brighter, cooler, and wetter environmental conditions. However, the sensitivity of GPP to an individual environmental variable was also altered by background meteorological gradients, whose changing pattern differed substantially among factors, indicating that the meteorological-regulated vegetation optimal photosynthetic range was a trade-off among heat, water, and light instead of being controlled by the univariable. This study implies that a deeper understanding of concurrent environmental variables is an effective way to reduce uncertainties in assessing the terrestrial carbon cycle perturbation exerted by human-induced emissions, especially under future scenarios with ongoing climate change.