Ocean acidification is projected to inhibit the biogenic production of calcium-carbonate skeletons in marine organisms. Antarctic waters represent a natural environment in which to examine the long-term effects of carbonate undersaturation on calcification in marine predators. King crabs (Decapoda: Anomura: Lithodidae), which currently inhabit the undersaturated environment of the continental slope off Antarctica, are potential invasives on the Antarctic shelf as oceanic temperatures rise. Here, we describe the chemical, physical, and mechanical properties of the exoskeleton of the deep-water Antarctic lithodid Paralomis birsteini and compare our measurements with two decapod species from shallow water at lower latitudes: Cancer borealis (Brachyura: Cancridae) and Callinectes sapidus (Brachyura: Portunidae). Paralomis birsteini deposit proportionally more calcium carbonate in their predatory chelae than their protective carapaces, compared with the other two crab species. When exoskeleton thickness and microhardness were compared between the chelae and carapace, the magnitude of the difference between these body regions was significantly greater in P. birsteini than in the other species tested. Hence, there appeared to be a greater disparity in P. birsteini in overall investment in calcium-carbonate structures among regions of the exoskeleton. The imperatives of prey consumption and predator avoidance may be influencing the deposition of calcium to different parts of the exoskeleton in lithodids living in an environment undersaturated with respect to calcium carbonate.