Mobile platform measurements provide new opportunities for characterizing spatial variations of air pollution within urban areas, identifying emission sources, and enhancing knowledge of atmospheric processes. The Aclima, Inc. mobile measurement and data acquisition platform was used to equip four Google Street View cars with research-grade instruments, two of which were available for the duration of this study. On-road measurements of air quality were made during a series of sampling campaigns between May 2016 and September 2017 at high (i.e., 1-second [s]) temporal and spatial resolution at several California locations: Los Angeles, San Francisco, and the northern San Joaquin Valley (including non-urban roads and the cities of Tracy, Stockton, Manteca, Merced, Modesto, and Turlock). The results demonstrate that the approach is effective for quantifying spatial variations of air pollutant concentrations over measurement periods as short as two weeks. Measurement accuracy and precision are evaluated using results of weekly performance checks and periodic audits conducted through the sampler inlets, which show that research instruments located within stationary vehicles are capable of reliably measuring nitric oxide (NO), nitrogen dioxide (NO2), ozone (O3), methane (CH4) black carbon (BC), and particle number (PN) concentration with bias and precision ranging from <10 % for gases to <25 % for BC and PN at 1-s time resolution. The quality of the mobile measurements in the ambient environment is examined by comparisons with data from an adjacent (< 9 m) stationary regulatory air quality monitoring site and by paired collocated vehicle comparisons, both stationary and driving. The mobile measurements indicate that U.S. EPA classifications of two Los Angeles stationary regulatory monitors' scales of representation are appropriate. Paired time-synchronous mobile measurements are used to characterize the spatial scales of concentration variations when vehicles were separated by <1 to 10 kilometers (km). A data analysis approach is developed to characterize spatial variations while limiting the confounding influence of diurnal variability. The approach is illustrated using data from San Francisco, revealing 1-km scale differences in mean NO2 and O3 concentrations up to 117 % and 46 %, respectively, of mean values during a two-week sampling period. In San Francisco and Los Angeles, spatial variations up to factors of 6 to 8 occur at sampling scales of 100 - 300m, corresponding to 1-minute averages.