Palatability of outer tissues of a suite (12 species) of Antarctic ascidians was evaluated using omnivorous fish and sea star predators. Tissues of 100% of those tested were unpalatable to fish, while 58% were unpalatable to sea stars. Lipophilic and hydrophilic extracts of 11 species were incorporated into pellets and tested in fish and sea star bioassays. Only the lipophilic extract from Distaplia colligans caused fish feeding deterrence. Organic extracts from 10 ascidian species were also examined in food pellet assays using an omnivorous amphipod. Only the lipophilic extract of D. cylindrica was a deterrent. Five of the ascidians possessed acidified outer tunics (pH < 3). We tested the ability of acidified krill pellets (pH 2 to 7) to deter fish and sea star predators and found that, while fish readily ingested acidified food pellets (pH 2), sea stars were deterred at pH 5 or less. Thus either organic or inorganic chemical defenses explain defense in 5 of the 7 ascidian species found unpalatable to sea stars. In contrast, chemical defenses only explain 1 of 12 species found unpalatable to fish, and only 1 of 10 ascidians tested against an amphipod predator. This predator-specific pattern of chemical defense may reflect greater predation pressure on ascidians from Antarctic sea stars. Alternatively, Antarctic ascidians may rely on other factors such as the toughness of their tunic or sequestration of heavy metals such as vanadium to inhibit feeding by Antarctic fish, a taxonomic group known to lack strong jaws. © Inter-Research 2009.