CO is a well-suited indicator for the transport of pollutants in the troposphere on a regional and global scale. For the study presented here, simulations of CO concentrations from a global chemistry transport model (MOZART-2), with the CO being tagged according to the emission type and the source region, have been used to diagnose the contributions of different processes and regions to the CO burden over Europe. Model simulations have been performed with both a priori emissions and an optimized set of CO surface emissions derived from the inversion of CO retrievals of the Measurements of Pollution in the Troposphere (MOPITT) remote sensing instrument. The annual mean difference between the modeled and the observed CO at 850 hPa over Europe is −38 ± 13 ppb with the a priori set of emissions and −7 ± 7 ppb when the optimized emissions are employed in the model. The general difficulties arising from an intercomparison of remote sensing data with model simulations are discussed. Besides data from MOPITT, ground-based CO measurements have been employed in the evaluation of the model and its emissions. The comparisons show that the model represents the background conditions as well as large-scale transport relatively well. The budget analysis reveals the predominant impact of the European emissions on CO concentrations near the surface, and a strong impact of sources from Asia and North America on the CO burden in the free troposphere over Europe. On average, the largest contribution (67%) to the anthropogenic (fossil and biofuel sources, biomass burning) CO at the surface originates from regional anthropogenic sources, but further significant impact is evident from North America (14%) and Asia (15%). With increasing altitude, anthropogenic CO from Asia and North America gains in importance, reaching maximum contributions of 32% for North American CO at 500 hPa and 50% for Asian CO at 200 hPa. The impact of European emissions weakens with increasing altitude (8% at 500 hPa).