In coastal ecosystems, top predators are exposed to a wide variety of nutrient and contaminant sources due to the diversity of trophic webs within coastal areas. Mercury contamination could represent an additional threat to shark populations that are declining worldwide. Here we measured total mercury, carbon and nitrogen isotopes as well as mercury isotopes in two co-occurring shark species (the bull shark Carcharhinus leucas and the tiger shark Galeocerdo cuvier) and their prey from a coastal ecosystem of the western Indian Ocean (La Réunion Island), to (i) determine their main trophic Hg source and (ii) better characterize their diet composition and foraging habitat. Hg isotope signatures (Δ199Hg and δ202Hg) of shark prey suggested that bull sharks were exposed to methylmercury (MeHg) produced in the water column while tiger sharks were exposed to mesopelagic MeHg with additional microbial transformation in slope sediments. Δ199Hg values efficiently traced the ecology of the two predators, demonstrating that bull sharks targeted coastal prey in shallow waters while tiger sharks were mainly foraging on mesopelagic species in the slope deeper waters. Unexpectedly, we found a positive shift in δ202Hg (>1‰) between sharks and their prey, leading to high δ202Hg values in the two shark species (e.g. 1.91 ± 0.52‰ in the bull shark). This large shift in δ202Hg indicates that sharks may display strong MeHg demethylation abilities, possibly reflecting evolutionary pathways for mitigating their MeHg contamination.