Au(core)-Ag(shell) triangular bifrustum nanocrystals were synthesized in aqueous solution using a seed-mediated approach. The formation of the Ag layer on the Au nanoprism seeds leads to structures with highly tunable dipole and quadrupole surface plasmon resonances. Discrete dipole approximation calculations show that it is the geometry of these novel structures rather than the addition of a new element that leads to the plasmon tunability. The structure and composition of these novel nanocrystals have been investigated by transmission electron microscopy, atomic force microscopy, X-ray photoelectron spectroscopy, and energy-dispersive spectrometry.