Marine amniotes have played many crucial roles in ocean ecosystems since the Triassic, including predation at the highest trophic levels. One genus often placed into this guild is the large Early Jurassic neoichthyosaurian Temnodontosaurus, the only post-Triassic ichthyosaurian known with teeth which bear a distinct cutting edge or carina. This taxonomically problematic genus is currently composed of seven species which show a wide variety of skull and tooth morphologies. Here we assess the craniodental disparity in Temnodontosaurus using a series of functionally informative traits. We describe the range of tooth morphologies in the genus in detail, including the first examples of serrated carinae in ichthyosaurians. These consist of false denticles created by the interaction of enamel ridgelets with the carinal keel, as well as possible cryptic true denticles only visible using scanning electron microscopy. We also find evidence for heterodonty in the species T. platyodon, with unicarinate mesial teeth likely playing a role in prey capture and labiolingually compressed, bicarinate distal teeth likely involved in prey processing. This type of heterodonty appears to be convergent with a series of other marine amniotes including early cetaceans. Overall, the species currently referred to as the genus Temnodontosaurus show a range of craniodental configurations allowing prey to be captured and processed in different ways – for example, T. eurycephalus has a deep snout and relatively small bicarinate teeth likely specialised for increased wound infliction and grip-and-tear feeding, whereas T. platyodon has a more elongate yet robust snout and larger teeth and may be more adapted for grip-and-shear feeding. These results suggest the existence of niche partitioning at higher trophic levels in Early Jurassic ichthyosaurians and have implications for future work on the taxonomy of this wastebasket genus, as well as for research into the ecology of other extinct megapredatory marine tetrapods.