This study combines advanced characterization techniques with conventional Charpy impact tests to relate the mechanical properties to the microstructure of technically pure molybdenum, especially regarding its toughness. V-notched samples with different orientations were prepared from a rolled molybdenum plate in stress-relieved and recrystallized condition. The ductile-tobrittle transition-temperature was analyzed in terms of the delamination behavior influenced by the microstructure. A pronounced increase of toughness was found for specific oriented samples, which can be explained by macroscopic delamination. Elongated grains led to enhanced delamination in Charpy impact tests with variations for different orientations. In general, delamination occurs as a result of brittle fracture; however, an increase in toughness in the Charpy impact test can be provoked. This mechanism is called thin sheet toughening or delamination toughening. Electron backscatter diffraction measurements were performed to get a deeper knowledge about crack propagation and delamination behavior in the rolled plate. Recrystallization shifts the transition region to significantly higher temperatures, which is explained by the globular grain shape as well as grain boundary segregation. The occurrence of delamination is discussed, taking texture, grain shape and segregation effects into account.