Negative trends of carbon monoxide (CO) concentrations are observed in the recent decade by both surface measurements and satellite retrievals over many regions, but they are not well explained by current emission inventories. Here, we attribute the observed CO concentration decline with an atmospheric inversion that simultaneously optimizes the two main CO sources (surface emissions and atmospheric hydrocarbon oxidations) and the main CO sink (atmospheric hydroxyl radical OH oxidation) by assimilating observations of CO and other chemically related tracers. Satellite CO column retrievals from Measurements of Pollution in the Troposphere (MOPITT), version 6, and surface in-situ measurements of methane and methyl-chloroform mole fractions are assimilated jointly for the period of 2002–2011. Compared to the prior simulation, the optimized CO concentrations show better agreement with independent surface in-situ measurements in terms of both distributions and trends. At the global scale, the atmospheric inversion primarily interprets the CO concentration decline as a decrease in the CO emissions, and finds noticeable trends neither in the chemical oxidation sources of CO, nor in the OH concentrations that regulate CO sinks. The latitudinal comparison of the model state with independent formaldehyde (CH 2 O) columns retrieved from the Ozone Measurement Instrument (OMI) confirms the absence of large-scale trends in the atmospheric source of CO. The global CO emission decreased by 17% during the decade, more than twice the negative trend estimated by emission inventories. The spatial distribution of the inferred decrease of CO emissions indicates contributions from both a decrease in fossil- and bio-fuel emissions over Europe, the USA and Asia, and from a decrease in biomass burning emissions in South America, Indonesia, Australia and Boreal regions. An emission decrease of 2% yr −1 is inferred in China, one of the main emitting regions, in contradiction with the bottom-up inventories that report an increase of 2% yr −1 during the study period. A large decrease in CO emission factors due to technology improvements would outweigh the increase of carbon fuel combustions and may explain the observed decrease. In Africa, instead of the negative trend (1% yr −1 ) reported by CO emission inventories mainly contributed by biomass burning, a positive trend (1.5% yr −1 ) is found by the atmospheric inversion, suggesting different trends between satellite-detected burned areas and CO emissions.