On-demand ridesourcing services from transportation network companies (TNCs), such as Uber and Lyft, have reshaped urban travel and changed externality costs from vehicle emissions, congestion, crashes, and noise. To quantify these changes, we simulate replacing private vehicle travel with TNCs in six U.S. cities. On average, we find a 50–60% decline in air pollutant emission externalities from NOx, PM2.5, and VOCs due to avoided “cold starts” and relatively newer, lower-emitting TNC vehicles. However, increased vehicle travel from deadheading creates a ∼20% increase in fuel consumption and associated greenhouse gas emissions and a ∼60% increase in external costs from congestion, crashes, and noise. Overall, shifting private travel to TNCs increases external costs by 30–35% (adding 32–37 ¢ of external costs per trip, on average). This change in externalities increases threefold when TNCs displace transit or active transport, drops by 16–17% when TNC vehicles are zero-emission electric, and potentially results in reduced externalities when TNC rides are pooled.