Among the fossiliferous sites of the Serra da Capivara national park region (South Eastern Piauí), two have yielded interesting remains of the two large Upper Pleistocene Carnivora, Protocyon troglodytes (Lund, 1838) and Smilodon populator Lund, 1842, the Toca da Cima dos Pilão and the Toca das Moendas, both in the municipality of Coronel José Dias. In these two caverns, numerous remains of preys were found, namely, for the Toca da Cima dos Pilão, the two peccaries Dicotyles tajacu and Tayassu pecari, the medium sized ground sloth Catonyx cuvieri and the giant armadillo Pampatherium; for the Toca das Moendas Palaeolama, Equids and Cervids add to that list. The two sites were used as dens by the two Carnivora species. In the Toca das Moendas, a near complete adult skull and a hemimandible of the large Canid P. troglodytes were found. The skull is the third ever known for the species. Its dimensions are very similar to those of a complete skull from the Toca da Boa Vista (Campo Formoso, Bahia, Brazil) described by Cartelle et Langguth (1999), and to those of an incomplete skull from the banks of the Bermejo River (Formosa Province, Argentina), described by Prevosti et al. (2005). It fits perfectly, like the teeth, with the anatomical characteristics of the species P. troglodytes: wide muzzle, short palate, very reduced and forwardly offset protocone of the P4/, etc. The dimensions of the cheek teeth correspond well with those of numerous teeth from Lagoa Santa (Minas Gerais, Brazil) of the Lund Collection preserved in the Zoological Museum of Copenhagen. The same site of Toca das Moendas yielded two left hemimandibles of the Machairodontine S. populator Lund, 1842, an adult and a very young ones. We study them together with other remarkable remains from the Toca da Cima dos Pilão, namely an adult upper canine and an adult hemimandible. The upper canine is one of the longest ever described for S. populator. The P/4 are somewhat longer than those of the Californian Smilodon fatalis (Leidy, 1868), and the M/1 are about of the same average length but somewhat narrower. The segment P/4-M/1 is relatively short. The dimensions of the upper canine and of the lower cheek teeth fit well with those of some teeth from Lagoa Santa (Minas Gerais, Brazil) and from Argentina preserved in the Zoological Museum of Copenhagen. We describe particularly the decidual lower dentition, badly known in that species. The rather weak milk canine has a piriform outline. The D/3 is constituted by a strong protoconid flanked with two small cuspids, an anterior and a posterior ones. The D/4 (deciduous carnassial) shows a strong paraconid followed by a higher protoconid and a small posterior cuspid. These milk teeth, without any abrasion mark, suggest that our young specimen was less than three month old.