In the present study, we investigated the concentrations and distributions of 57 anthropogenic pollutants, including 23 organochlorine pesticides (OCs), 18 polychlorinated biphenyls (PCBs) and 16 polycyclic aromatic hydrocarbons (PAHs) in liver samples from 102 birds of prey of six species that were found dead or that had died during their stay in the Wildlife Recovery Centers of the Canary Islands (Spain) between 2009 and 2012. The dual goal of this work was to determine the occurrence of these contaminants in these six species of birds of prey, and also whether they can be used as bioindicators for monitoring environmental pollution in the region. We found that Accipiter nisus, Falco pelegrinoides and Falco tinnunculus were the most contaminated species. The profiles of contamination among the species were extremely similar in the case of organochlorine contaminants, with DDT and its metabolites as the most abundant compounds. The contamination by DDT and its metabolites, as well as contamination by dieldrin, could be considered high in these animals, much higher than reports from other regions of the planet, which is in agreement with previous reports from our group regarding humans, food and other animals from this area. In contrast, the contamination by PCBs could be considered extremely low and was probably below the threshold of toxicity for these contaminants. The content of carcinogenic/mutagenic PAHs in these animals was clearly dependent on the feeding pattern of the species; however, the levels were also well below the values that were considered toxic in predictive models. This study represents the first report of contamination by PAHs in all these species and is also the first report of PCB levels in Barbary Falcons.