To assess the feasibility of using animal excrement to biomonitor the extent of heavy metal contamination in the marine environment, concentrations of mercury (Hg), lead (Pb), copper (Cu) and zinc (Zn) in the fresh excrement of seabirds and marine mammals, along with other biomaterials, from the Arctic, Antarctica (West and East), and Xisha Archipelago of the South China Sea were determined. ... Results show that the excrement of marine animals at higher trophic levels generally contained high levels of Hg, demonstrating the biomagnification of Hg through food chains in different remote regions. Significant variations in metal accumulation in the excrements were observed among the distinctive geographical areas, with the highest Hg concentration in Xisha Archipelago and the highest Pb concentration in the Arctic, which reflects different levels of air metal pollution at various sampling locations. Concentrations of Cu in the excrements primarily correlate to the geochemical background levels in the regions. High Cu concentrations were found near the Great Wall Station in West Antarctica where a copper mineralized belt exists. No clear spatial variation pattern was found for Zn accumulation in the excrement. This study shows that animal excrement can be used as bioindicators for the level of metal contamination in the marine environment, with the advantages of easy sampling, accurate detection (i.e., with high levels of metal accumulation), and reconstructing historical metal contamination trends by long-term monitoring of sedimentary excrements.