Vertebrate teeth are complex structures adapted in terms of shape and structure to serve a variety of functions like biting and grinding. Thus, examining the morphology, composition and mechanical properties of the teeth can aid in providing insights into the feeding behaviour of extinct species. We here provide the first mechanical characterisation of teeth in a spinosaurid dinosaur, Suchomimus tenerensis, and a pholidosaurid crocodylomorph, Sarcosuchus imperator. Our results show that both species have similar macrostructure of enamel, dental and interfacial layers, and similar composition, the main constituent being fluoroapatite. Microindentation tests show that Suchomimus teeth have lower elastic modulus and hardness, as compared to Sarchosuchus. On the contrary, Sarcosuchus teeth have lower toughness. Nanoindentation showed the existence of mechanical gradients from dentin to enamel in Suchomimus and, less prominently, in Sarcosuchus. This was also supported by wear tests showing that in Suchomimus the dentin region is more wear-prone than the enamel region. With still scarce information available on the dietary regimes in extinct species the analysis of micro and nano-mechanical properties of fossils teeth might be a help in targeting specific biological questions. However, much is still unknown concerning the changes underwent by organic material during diagenesis making at present impossible to definitely conclude if the differences in the mechanical properties of Suchomimus and Sarchosuchus here retrieved imply that the two species adopted different strategies when dealing with food processing or are the result of disparate taphonomic histories.