Laves-type intermetallic phases have been observed to be the dominant phases in a series of alloy compositions being designed for the immobilization of technetium in a metallic waste form. The dominant metals in the alloy compositions were Fe-Mo and Fe-Mo-Zr. The alloy composition, Fe-Mo-Zr, also contained Pd, Zr, Cr, and Ni. Both non-radioactive rhenium-containing and radioactive technetium-bearing alloy compositions were investigated. In the Fe-Mo series, the phases observed were Fe2Mo (C14 Laves phase) and ferrite in agreement with predictions. Both Tc and Re resided predominantly in the Laves phases. In the Fe-Mo-Zr system, the phases included hexagonal C14 with the composition (Fe,Cr)2Mo, cubic C15 phase with a (Fe,Ni)2Zr composition, and the hcp phase Pd2Zr. The observation of these phases was in agreement with predictions. Re was found in the C14 intermetallic, (Fe,Cr)2Mo. Technetium was also observed to be partitioned preferentially into the (Fe,Cr)2Mo phase; however, this phase exhibited a cubic structure consistent with the C15 structural type. The composition of Laves phases is influenced by both the atomic size and electro-negativity of the constituent elements. The long-term release behavior of technetium under nuclear waste disposal conditions may be more dependent on the corrosion characteristics of these individual Laves phases containing Tc than the other metallic phases.