Modern high Charpy toughness steels can nonetheless show low crack arrest toughness. In this paper, the relationship between initiation and arrest toughness is investigated in five different carbon steels, including S355 structural steels, X65 pipeline steel, and high strength reactor pressure vessel, RPV, steels. The results from small-scale mechanical tests, including instrumented Charpy, drop weight Pellini, fracture toughness, and tensile testing (including STRA in the through-thickness direction) were used to determine the behaviour of the different steels in terms of initiation fracture toughness and crack arrest toughness parameters. There was no correlation between the upper shelf initiation toughness and the arrest toughness when the results from the five steels were collated. The mechanical test results were then correlated to the steels’ microstructural characteristics, including parent metal microstructure, average grain size and grain aspect ratio to identify the relative roles of microstructure and texture in the fracture initiation and arrest performance of carbon steels.