Synoptic variations of atmospheric CO<sub>2</sub> produced by interactions between weather and surface fluxes are investigated mechanistically and quantitatively in midlatitude and tropical regions using continuous in-situ CO<sub>2</sub> observations in North America, South America and Europe and forward chemical transport model simulations with the Parameterized Chemistry Transport Model. Frontal CO<sub>2</sub> climatologies show consistently strong, characteristic frontal CO<sub>2</sub> signals throughout the midlatitudes of North America and Europe. Transitions between synoptically identifiable CO<sub>2</sub> air masses or transient spikes along the frontal boundary typically characterize these signals. One case study of a summer cold front shows CO<sub>2</sub> gradients organizing with deformational flow along weather fronts, producing strong and spatially coherent variations. In order to differentiate physical and biological controls on synoptic variations in midlatitudes and a site in Amazonia, a boundary layer budget equation is constructed to break down boundary layer CO<sub>2</sub> tendencies into components driven by advection, moist convection, and surface fluxes. This analysis suggests that, in midlatitudes, advection is dominant throughout the year and responsible for 60–70% of day-to-day variations on average, with moist convection contributing less than 5%. At a site in Amazonia, vertical mixing, in particular coupling between convective transport and surface CO<sub>2</sub> flux, is most important, with advection responsible for 26% of variations, moist convection 32% and surface flux 42%. Transport model sensitivity experiments agree with budget analysis. These results imply the existence of a recharge-discharge mechanism in Amazonia important for controlling synoptic variations of boundary layer CO<sub>2</sub>, and that forward and inverse simulations should take care to represent moist convective transport. Due to the scarcity of tropical observations at the time of this study, results in Amazonia are not generalized for the tropics, and future work should extend analysis to additional tropical locations.