High uncertainties affect black carbon (BC) emissions , and, despite its important impact on air pollution and climate, very few BC emissions evaluations are found in the literature. This paper presents a novel approach, based on airborne measurements across the Paris, France, plume, developed in order to evaluate BC and NO x emissions at the scale of a whole agglomeration. The methodology consists in integrating, for each transect, across the plume observed and simulated concentrations above background. This allows for several error sources (e.g., representativeness, chemistry, plume lateral dispersion) to be minimized in the model used. The procedure is applied with the CHIMERE chemistry-transport model to three inventories-the EMEP inventory and the so-called TNO and TNO-MP inventories-over the month of July 2009. Various systematic uncertainty sources both in the model (e.g., boundary layer height, vertical mixing , deposition) and in observations (e.g., BC nature) are discussed and quantified, notably through sensitivity tests. Large uncertainty values are determined in our results, which limits the usefulness of the method to rather strongly erroneous emission inventories. A statistically significant (but moderate) overestimation is obtained for the TNO BC emissions and the EMEP and TNO-MP NO x emissions, as well as for the BC / NO x emission ratio in TNO-MP. The benefit of the airborne approach is discussed through a comparison with the BC / NO x ratio at a ground site in Paris, which additionally suggests a spatially heterogeneous error in BC emissions over the agglomeration.