We evaluated the presence of 37 organohalogen contaminants in plasma samples from 162 juvenile and 197 adult loggerhead turtles (Caretta caretta) from the archipelagos of the Canary Islands and Cape Verde, respectively, and compared the contamination profiles found. We detected five organochlorine pesticides (OCP) and 16 polychlorinated biphenyls (PCBs). The concentrations of the two groups of contaminants were higher in turtles from the Canary Islands (OCPs, 1.04 vs. 0.37 ng/mL; PCBs, 1.92 vs. 0.08 ng/mL). We also observed a different profile of PCB contamination between the two populations. In addition, there was a negative correlation between body size and the total concentration of PCBs in the Canary Islands turtles, but not in turtles from Cape Verde. The present study presents the first data on the organochlorine contaminants (OCs) of live turtles from Canary Islands. In addition, we perform a comparison of the levels and profiles of OCs between these two different groups of loggerhead sea turtles from the Eastern Atlantic.