The Nano Aerosol Mass Spectrometer (NAMS) was deployed to the California Nexus Los Angeles ground site in Pasadena, California during May–June 2010 to study nanoparticles in the 20–25 nm size range. NAMS gives a quantitative measure of the elemental composition of individual particles, and molecular apportionment of the elemental data allows the O/C mole ratio of carbonaceous matter in each particle to be determined. Abrupt increases in nanoparticle number concentration were observed in the afternoon on sunny days, and coincided with a shift in the wind direction from the southeast to the southwest. Nanoparticles analyzed during these time periods were found to contain enhanced levels of sulfur and silicon relative to particles analyzed earlier in the day, and the O/C ratios of carbonaceous matter changed from a distribution dominated by primary motor vehicle emissions (O/C ratio < 0.25) to one dominated by “fresh” secondary organic aerosol (O/C ratio between 0.25 and 0.65). The wind direction and chemical composition dependencies suggest that the afternoon increase in number concentration originated from motor vehicle emissions in the downtown Los Angeles area that were photochemically processed during transport to the measurement site. It is likely that photochemical processing led to both a change in the composition of preexisting particles and to the formation of new particles.