The fossil came from a pliosaur, a ferocious predator that lived in the oceans 150 million years ago.
The skull was discovered in Dorset by a collector and measures 2.4m in length. The discovery was announced on Tuesday.
Scientists believe the creature would have been about 16 metres long.
David Martill, a paleontologist from the University of Portsmouth, says pliosaurs had short necks and huge, crocodile-like heads with powerful jaws and a set of razor-sharp teeth.
He said they used paddle-like limbs to propel their bodies through the water and were generally carnivores.
The skull will be put on display in a Dorset museum.