A fitting method using a semi-empirical Gaussian dispersion model solution was successfully applied to obtain both dispersion coefficients and a particle number emission factor (PNEF) directly from ultrafine particle (UFP; particles smaller than <0.1 μm in diameter) concentration profiles observed downwind of major roadways in California's South Coast Air Basin (SoCAB). The effective Briggs' formulation for the vertical dispersion parameter σ_z was adopted in this study due to its better performance in describing the observed profiles compared to other formulations examined. The two dispersion coefficients in Briggs' formulation, α and β, ranged from 0.02 to 0.07 and from −0.5 × 10⁻³ to 2.8 × 10⁻³, respectively, for the four freeway transects studied and are significantly different for freeways passing over vs. under the street on which measurements of the freeway plume were made. These ranges are wider than literature values for α and β under stable conditions. The dispersion coefficients derived from observations showed strong correlations with both surface meteorology (wind speed/direction, temperature, and air stability) and differences in concentrations between the background and plume peak. The relationships were applied to predict freeway plume transport using a multivariate regression, and produced excellent agreement with observed UFP concentration profiles. The mean PNEF for a mixed vehicle fleet on the four freeways was estimated as 7.5 × 10¹³ particles km⁻¹ vehicle⁻¹, which is about 15% of the value estimated in 2001 for the I-405 freeway, implying significant reductions in UFP emissions over the past decade in the SoCAB.