The Long Island Sound Tropospheric Ozone Study (LISTOS) was organized to investigate ozone formation and transport in the New York City metropolitan area and locations downwind. During LISTOS, the University at Albany Atmospheric Sciences Research Center (ASRC) mobile laboratory was used for measuring surface O3, NO2, and aerosol number and mass concentration. Sharp O3 concentration gradients, with ΔO3 Δy−1 over 15 ppb km−1, were measured both at and near the land‐water interface and on the highway on days characterized by high regional O3 concentrations. These large O3 gradients at or near the land‐water interface, and in air masses relatively low in NO2, are shown to be influenced in part by the transport of highly oxidized air masses via sea breeze circulation and convergence with gradient flow. On the highway under regionally high O3 concentrations, strong anticorrelation (R2 = 0.78, p < 0.05) between O3 and NO2 and an absolute slope less than 1 suggested that Ox concentrations (O3 + NO2) increased with increasing NO2. Overall, the on‐road measurements made during LISTOS help to better characterize the interaction between the emitted pollution and the meteorological conditions on Long Island, thereby having potential policy implications.