Objectives. To quantify health benefits and carbon emissions of 2 transportation scenarios that contrast optimum levels of physical activity from active travel and minimal air pollution from electric cars. Methods. We used data on burden of disease, travel, and vehicle emissions in the US population and a health impact model to assess health benefits and harms of physical activity from transportation-related walking and cycling, fine particulate pollution from car emissions, and road traffic injuries. We compared baseline travel with walking and cycling a median of 150 weekly minutes for physical activity, and with electric cars that minimized carbon pollution and fine particulates. Results. In 2050, the target year for carbon neutrality, the active travel scenario avoided 167 000 deaths and gained 2.5 million disability-adjusted life years, monetized at $1.6 trillion using the value of a statistical life. Carbon emissions were reduced by 24% from baseline. Electric cars avoided 1400 deaths and gained 16 400 disability-adjusted life years, monetized at $13 billion. Conclusions. To achieve carbon neutrality in transportation and maximize health benefits, active travel should have a prominent role along with electric vehicles in national blueprints. (Am J Public Health. 2022; 112(3):426-433. https://doi.org/10.2105/AJPH.2021.306600).