Abstract. In this paper we investigate the atomic structure and composition of grain boundaries in Cu3Au (weakly ordered compound) and Ni3AI (strongly ordered compound). Computer simulations employing both the molecular statics and Monte Carlo methods were performed and the Finnis-Sinclair type many-body central force potentials used. First, grain boundaries in stoiehiometric alloys are studied with the goal to investigate the impact of ordering strength on the grain boundary structure and composition. In Cu3Au grain boundaries may become compositionally disordered even at room temperature and the compositional disordering is associated with segregation of gold. In contrast, in Ni3A1 grain boundaries remain compositionally ordered up to very high temperatures. Secondly, the structures of grain boundaries and the effect of Ni and AI segregation in non-stoichiometric Ni3A1 are investigated. Nickel segregation leads to compositional disordering at grain boundaries, while aluminum segregation, which is strongly selective, leads to an ordered grain boundary structure with high AI content. The possible relationship between structural and compositional characteristics of grain boundaries and their mechanical properties, in particular the grain boundary brittleness and its alleviation by additional alloying, are then discussed in the light of the results of this study.