Vehicles are a major source of anthropogenic emissions of carbon monoxide (CO), nitrogen oxides (NOx), and black carbon (BC). CO and NOx are known to be harmful to human health and contribute to ozone formation, while BC absorbs solar radiation that contributes to global warming and also has negative impacts on human health and visibility. Travel restrictions implemented during the COVID-19 pandemic provide researchers the opportunity to study the impact of large, on-road traffic reductions on local air quality. Traffic counts collected along Interstate-95, a major eight-lane highway in Maryland (US), reveal a 60% decrease in passenger car totals and an 8.6% (combination-unit) and 21% (single-unit) decrease in truck traffic counts in April 2020 relative to prior Aprils. The decrease in total on-road vehicles led to the near-elimination in stop-and-go traffic and a 14% increase in the mean vehicle speed during April 2020. Ambient near-road (NR) BC, CO, NOx, and carbon dioxide (CO2) measurements were used to determine vehicular emission ratios (ΔBC/ΔCO, ΔBC/ΔCO2, ΔNOx/ΔCO, ΔNOx/ΔCO2, and ΔCO/ΔCO2), with each ratio defined as the slope value of a linear regression performed on the concentrations of two pollutants within an hour. A decrease of up to a factor of two in ΔBC/ΔCO, ΔBC/ΔCO2, ΔNOx/ΔCO2, and in the fraction of on-road diesel vehicles from weekdays to weekends shows diesel vehicles to be the dominant source of BC and NOx emissions at this NR site. We estimate up to a 70% reduction in BC emissions in April 2020 compared to earlier years, and attribute much of this to lower diesel BC emissions resulting from improvements in traffic flow and fewer instances of acceleration and braking. Future efforts to reduce vehicular BC emissions should focus on improving traffic flow or turbocharger lag within diesel engines. Inferred BC emissions from the NR site also depend on ambient temperature, with an increase of 54% in ΔBC/ΔCO from −5 to 20 °C during the cold season, similar to previous studies that reported increasing BC emissions with rising temperature. The default setting of MOVES3, the current version of the mobile emission model used by the US EPA, does not adjust hot-running BC emissions for ambient temperature. Future work will focus on improving the accuracy of mobile emissions in air quality modeling by incorporating the effects of temperature and traffic flow in the system used to generate mobile emissions input for commonly used air quality models.