Among the three recognized species of Smilodon, S. populator is the largest in size and has the widest distribution across South America. The present contribution describes an almost complete skull assigned to the aforementioned felid. The material was recovered from sediments of the Dolores Formation (Lujanian Stage/Age) from the southern part of Uruguay. This specimen is remarkable for its unusual craniodental measurements, indicating that it is one of the largest known specimens of the genus.