We have performed a first-principles computational tensile test on an aluminum grain boundary (GB) with sulfur segregation. We show that the tensile strength is reduced by 18% (to 7.80 GPa) due to sulfur segregation in comparison with 9.50 GPa of the clean GB, and the GB fracture is caused by the interfacial bond breaking. We demonstrate the peculiar behavior of a sulfur-aluminum atom cluster at the interface during the tensile test, which originates from the intrinsic bonding characteristic of sulfur. Such cluster forms a one-dimensional chain structure that is similar to that in the bulk S, and remains unchanged in the tensile process until the fracture occurs but significantly changes the GB structure. This is responsible for the observed fact that the segregated sulfur atom bonds strongly with only a few of its neighboring aluminum atoms, leading to weaker interfacial aluminum-sulfur bonds. We suggest that the experimentally observed aluminum intergranular embrittlement is induced by the GB weakening due to sulfur segregation.