Au/Pd octopods, nanostructures with eight branches and a primarily 750 Au interior, have been synthesized as size-controlled samples through the manipulation of seed-mediated co-reduction. The position of their localized surface plasmon resonance can be controllably tuned throughout the visible and near-infrared regions, and this response is correlated with the structural features (branch length and tip width) of the octopods. These Au/Pd octopods were also found to be highly sensitive to changes in the local refractive index of the surrounding media and suitable substrates for surface enhanced Raman spectroscopy. These findings, coupled with their unique composition, highlight the multifunctional capabilities of the Au/Pd octopods and provide insight into the optical properties of architecturally controlled bimetallic nanostructures.