Following the end-Cretaceous mass extinction, mammals underwent an increase in body size, taxonomic diversity and ecological specialization throughout the Paleocene, exemplifying their adaptability. One especially enigmatic group is the “Triisodontidae”, medium- to large-sized ungulate-like placentals from the Paleocene which are best known from their teeth that exhibit adaptations towards carnivory. The “triisodontids” were the first large carnivorous mammals and pre-date, and may have given rise to, Mesonychia, a group of more specialized placental carnivores. The “triisodontids” have been well-described from dental material, although very little is known about their postcrania. Here, we describe the postcrania of Triisodon crassicuspis–the most completely represented species of the genus to date–from a specimen (NMMNH P-72096) recovered from basal Torrejonian strata of the Nacimiento Formation in the San Juan Basin, New Mexico. Anatomical comparisons reveal that the forelimb long bones of Tri. crassicuspis are robust relative to its size, more so than other “triisodontids”. Attachment sites on the ulna are evidence of well-developed muscles involved in powerful extension and flexion of the manus. In Tri. crassicuspis, the range of pronation-supination was limited as evident from the humeroradial morphology. Qualitative functional assessment of osteological features of the forelimb of Tri. crassicuspis is suggestive of terrestrial locomotion with at least moderate digging ability. Re-analyses of the dentition confirmed that Tri. crassicuspis had specializations for carnivory, and provide a body mass estimate of ca. 32–44 kg based on dental proxies. In summary, Tri. crassicuspis was a relatively large and powerful terrestrial animal, and one of the first known placentals to fill a largely carnivorous niche.