Incorporating metallic nanostructures into dye-sensitized solar cells (DSSCs) is shown to increase light harvesting efficiency by coupling light from the far-field to the near-field, where it can be readily absorbed by molecular chromophores. In order to optimize this system, core-shell-shell nanoparticles along with a nanostructured aggregate architecture have been developed and are shown to significantly improve DSSC efficiency by concentrating light via surface plasmon resonance. Aggregates are shown to absorb light strongly throughout the visible light region and increase overall efficiency from 2.81% to 5.52%, while coreshell-shell nanoparticles are studied to determine the basic processes of plasmonic DSSCs. Comparisons between experimental data and theoretical calculations provide further insight into the structure of the nanoparticles and solar cells made using them. This guides our synthetic approach and aids in our understanding of the nature of plasmonic enhancement in solar cells.