The causes of internal cracking that occurred in 9% Ni steel castings during manufacture were investigated using a series of eight laboratory castings containing varying amounts of molybdenum. The effect of mold thickness was also investigated. The laboratory castings were subjected to three-point bend testing, and fracture surfaces were examined using SEM fractography, metallography, and depth analysis (SIMS) of the fracture surface. The cracks were found to originate at austenitic grain boundaries that coincided with primary dendrite interfaces. The cracking was attributed to a decrease in grain-boundary cohesion resulting from sulfur segregation. Addition of molybdenum proved effective in preventing cracking. The molybdenum promoted MnS precipitation in the grain and preferentially segregated to the interfaces.