The electronic structure of single crystal UO2 and polycrystalline δ-Pu is examined using photoelectron spectroscopy. These two actinide materials exhibit properties consistent with the 5f electrons at the threshold between localized and itinerant character. The results for δ-Pu may be viewed as the 5f electrons exhibiting a dual nature with some fraction of the 5f levels localized and not participating in the bonding while the other fraction of 5f character is involved in bonding and hybridization with the conduction electrons. For UO2 where angle-resolved photoemission is available, one observes dispersion in the 5f features indicative of the 5f electrons being influenced by the periodic potential of the lattice rather than purely influenced by the site to which the 5f electrons are generally localized.