Mercury, a toxic metal released by various human activities, exerts environmental stress through its bioaccumulation and biomagnification, particularly in marine habitats. South American fur seals (Arctocephalus australis) and sea lions (Otaria flavescens) reproduce on the Atlantic coast of Uruguay. As top predators, they can accumulate toxic levels of mercury and are often used as sentinel species for monitoring ecosystem health. Fur seals prey on pelagic species, such as fish and squid, while sea lions consume coastal-benthic prey. We analyzed the total mercury concentration (THg) in hair and the trophic habits (δ 13 C and δ 15 N) of females from both species. The average THg concentration in adult female sea lions (30.5 ± 9.3 μg/g dry weight) was significantly higher than in fur seals (6.3 ± 2.5 μg/g dry weight). Additionally, the mean δ 15 N and δ 13 C values were significantly higher in sea lion (δ 15 N: 19.2 ± 0.6‰, δ 13 C: -13.8 ± 0.2‰) compared to fur seals (δ 15 N: 16.5 ± 0.5‰, δ 13 C: -15.5 ± 0.6‰). Our results suggest that different trophic levels and feedings areas affect the THg concentration in Uruguayan Otariids. Notably, at the intraspecific level, the THg concentration in sea lions increased with δ 13 C values, suggesting a link to coastal feeding habits. This indicates that coastal feeding behaviors, compared to feeding in pelagic environments, enhance mercury bioaccumulation in Otariids along the Uruguayan coast, with the discharge of freshwater from the Río de la Plata (one of the largest estuaries in South America) basin identified as a potential mercury source. THg concentrations found in female sea lion hair are the highest reported in Otariids globally. Mercury levels exceeded toxic thresholds observed in other mammals and could pose significant health risks. Our findings may explain why sea lions were particularly affected by the avian influenza outbreak in Uruguay compared to fur seals. Monitoring the declining sea lion population is crucial, making our results significant for integrated conservation and management strategies.