In this thesis, I demonstrate the rational design and controllable fabrication of a series of novel plasmonic nanostructures with judiciously tailored optical properties including perfect nanoshells, roughened subwavelength particles, prolate nanoshells known as nanorice, and non-concentric nanoshells known as nanoeggs. All of these nanostructures are very important subwavelength nanoscale optical components that can be utilized to manipulate light in unique ways. The most striking feature of these nanoparticles is their geometrically tunable plasmon resonances, which can be harnessed for widespread applications. I have also utilized these nanostructures as the building blocks to construct self-assembled multinanoparticle systems, such as nanoshell heterodimers, nanosphere arrays and nanoshell arrays. I have further developed multifunctional molecular sensing platforms using these nanoengineered plasmonic structures as substrates for surface-enhanced spectroscopies, realizing integrated analytical chemistry lab-on-a-chip. Applying the Plasmon Hybridization model as design principles to experimentally realizable nanostructures results in a thorough understanding of the origin of the geometry-dependent optical properties observed in these nanosystems. Finite Difference Time Domain (FDTD) method also provides a powerful platform for the numerical simulation of local- and far-field optical properties of these nanostructures.