Mesozoic mammals are commonly portrayed as shrew- or rat-sized animals that were mainly insectivorous, probably nocturnal and lived in the shadow of dinosaurs. The largest known Mesozoic mammal represented by substantially complete remains is Repenomamus robustus, a triconodont mammal from the Lower Cretaceous of Liaoning, China. An adult individual of R. robustus was the size of a Virginia opossum. Here we report a new species of the genus, represented by a skeleton with most of the skull and postcranium preserved in articulation. The new species is 50% larger than R. robustus in skull length. In addition, stomach contents associated with a skeleton of R. robustus reveal remains of a juvenile Psittacosaurus, a ceratopsian dinosaur. Our discoveries constitute the first direct evidence that some triconodont mammals were carnivorous and fed on small vertebrates, including young dinosaurs, and also show that Mesozoic mammals had a much greater range of body sizes than previously known. We suggest that Mesozoic mammals occupied diverse niches and that some large mammals probably competed with dinosaurs for food and territory.