This study assessed the spatial variability of PM2.5 source contributions across ten sites located in the South Coast Air Basin, California. Eight pollution sources and their contributions were obtained using positive matrix factorization (PMF) from the PM2.5 compositional data collected during the two sampling campaigns (2012/13 and 2018/19) of the Multiple Air Toxics Exposure Study (MATES). The identified sources were “gasoline vehicles”, “aged sea salt”, “biomass burning”, “secondary nitrate”, “secondary sulfate”, “diesel vehicles”, “soil/road dust” and “OP-rich”. Among them, “gasoline vehicle” was the largest contributor to the PM2.5 mass. The spatial distributions of source contributions to PM2.5 at the sites were characterized by the Pearson correlation coefficients as well as coefficients of determination and divergence. The highest spatial variability was found for the contributions from the “OP-rich” source in both MATES campaigns suggesting varying influences of the wildfires in the Los Angeles Basin. Alternatively, the smallest spatial variabilities were observed for the contributions of the “secondary sulfate” and “aged sea salt” sources resolved for the MATES campaign in 2012/13. The “soil/road dust” contributions of the sites from the 2018/19 campaign were also highly correlated. Compared to the other sites, the source contribution patterns observed for Inland Valley and Rubidoux were the most diverse from the others likely due to their remote locations from the other sites, the major urban area, and the Pacific Ocean.