A fuel-based approach is used to estimate long-term trends (1990-2010) in carbon monoxide (CO) emissions from motor vehicles. Non-methane hydrocarbons (NMHC) are estimated using ambient NMHC/CO ratios after controlling for nonvehicular sources. Despite increases in fuel use of ∼10-40%, CO running exhaust emissions from on-road vehicles decreased by ∼80-90% in Los Angeles, Houston, and New York City, between 1990 and 2010. The ratio of NMHC/CO was found to be 0.24 ± 0.04 mol C/mol CO over time in Los Angeles, indicating that both pollutants decreased at a similar rate and were improved by similar emission controls, whereas on-road data from other cities suggest rates of reduction in NMHC versus CO emissions may differ somewhat. Emission ratios of CO/NOx (nitrogen oxides = NO + NO2) and NMHC/NOx decreased by a factor of ∼4 between 1990 and 2007 due to changes in the relative emission rates of passenger cars versus diesel trucks, and slight uptick thereafter, consistent across all urban areas considered here. These pollutant ratios are expected to increase in future years due to (1) slowing rates of decrease in CO and NMHC emissions from gasoline vehicles and (2) significant advances in control of diesel NOx emissions.