A new approach to the design of Ni-based polycrystalline superalloys is proposed. It is based on a concept that under given structural conditions, the performance of superalloys is determined by the strength of interatomic bonding both in the bulk and at grain boundaries of material. We characterize the former by the cohesive energy of the bulk alloy, whereas for the latter we employ the work of separation of a representative high angle grain boundary. On the basis of our first principle calculations we suggest Hf and Zr as “minor alloying additions” to Ni-based alloys. Re, on the other hand, appears to be of little importance in polycrystalline alloys.