Atoposaurids were a clade of semiaquatic crocodyliforms known from the Late Jurassic to the latest Cretaceous. Tentative remains from Europe, Morocco, and Madagascar may extend their range into the Middle Jurassic. Here we report the first unambiguous Middle Jurassic (late Bajocian–Bathonian) atoposaurid: an anterior dentary from the Isle of Skye, Scotland, UK. A comprehensive review of atoposaurid specimens demonstrates that this dentary can be referred to Theriosuchus based on several derived characters, and differs from the five previously recognized species within this genus. Despite several diagnostic features, we conservatively refer it to Theriosuchus sp., pending the discovery of more complete material. As the oldest known definitively diagnostic atoposaurid, this discovery indicates that the oldest members of this group were small-bodied, had heterodont dentition, and were most likely widespread components of European faunas. Our review of mandibular and dental features in atoposaurids not only allows us to present a revised diagnosis of Theriosuchus, but also reveals a great amount of variability within this genus, and indicates that there are currently five valid species that can be differentiated by unique combinations of dental characteristics. This variability can be included in future broad-scale cladistics analyses of atoposaurids and closely related crocodyliforms, which promise to help untangle the complicated taxonomy and evolutionary history of Atoposauridae.