Vaults are large protein nanocapsules that may be useful as drug delivery vehicles due to their normal presence in humans, their large interior volume, their simple structural composition consisting of multiple copies of one protein, and a recombinant production system that also provides a means to tailor their structure. However, for vaults to be effective in such applications, efficient means to load the interiors of the capsules must be demonstrated. Here we describe the use of a domain derived from a vault lumen-associated protein as a carrier to target both gold nanoclusters and heterologous His-tagged proteins to specific binding sites on the vault interior wall.