To investigate the relationship among sources, chemical composition, and redox activity of coarse particulate matter (CPM), three sampling sites were set up up in the Los Angeles Basin to collect ambient coarse particles at four time periods (morning, midday, afternoon, and overnight) in summer 2009 and winter 2010. The generation of reactive oxygen species (ROS) was used to assess the redox activity of these particles. Our results present distinct diurnal profiles of CPM-induced ROS formation in the two seasons, with much higher levels in summer than winter. Higher ROS activity was observed in the midday/afternoon during summertime, while the peak activity occurred in the overnight period in winter. Crustal materials, the major component of CPM, demonstrated very low water-solubility, in contrast with the modestly water-soluble anthropogenic metals, including Ba and Cu. The water-soluble fraction of four elements (V, Pd, Cu, and Rh) with primary anthropogenic origins displayed the highest associations with ROS activity (R(2) > 0.60). Our results show that coarse particles generated by anthropogenic activities, despite their low contribution to CPM mass, are important to the biological activity of CPM, and that a more targeted control strategy may be needed to protect the public health from these toxic CPM sources.