The relationship between black carbon (BC) and carbon monoxide (CO) has been analyzed using measurements from two sites in Mexico City and five urban areas in Germany. The correlation coefficient between BC and CO is greater than 0.90 for all sites. The average slope of the linear regression line for BC versus CO is 2.2 μg mg−1 for German sites and 1.1 μg mg−1 in Mexico City. The most important factors that affect the BC to CO relationship appear to be the ratio of diesel to gasoline usage and the combustion efficiency of vehicles in a particular area. The results of this analysis suggest that CO measurements in urban areas can be used to estimate BC mass when direct measurements are not available.