Two-phase intermetallic alloys composed of geometrically close packed (GCP) Ni3Al (L12 phase) and Ni3V (D022 phase) have attractive mechanical properties at high temperature, and are therefore considered to be used as high temperature structural materials. In this study, the effect of Ta and Re addition on the microstructure and hardness of two-phase intermetallic alloys was investigated. The addition of Ta remarkably enhanced the hardness due to solid solution hardening of the constituent phases. On the other hand, the addition of Re retarded the formation of the two-phase microstructure, resulting in the lowest hardness in the solution treated condition. By aging at 1223 K, the Ni solid solution in the Re added alloy decomposed to Ni3Al and Ni3V, accompanied by precipitates of a Re-rich phase. Consequently, the hardness rapidly increased with increasing aging time. Simultaneous addition of Ta and Re induced very fine precipitates of a Re-rich phase after aging, and consequently resulted in a higher hardness than by the addition of Ta or Re alone.