As an alternative technique, electroless deposition is gaining interest due to its simplicity (solution-based process, no complex instrumentation), economical aspect, and effectiveness to form certain desired film thicknesses and morphologies on a wide variety of substrates. This work describes the use of water-soluble, polyvalent star polymer templates to form spontaneous self-limiting monolayers on complimentary functionalized substrates that act as efficient adhesion layers for the electroless deposition of thin gold films. The resulting gold films display outstanding thickness control, uniformity, reproducibility, and plasmon resonance generation, as evaluated by Rutherford backscattering spectroscopy (RBS), surface plasmon resonance (SPR) spectroscopy, and atomic force microscopy (AFM). The adaptation of this technique to the formation of core-shell gold nanoparticles was also shown to be feasible. The synthesized star polymer-templated gold nanoshells display a tunable NIR absorption depending on their size. By utilizing star polymers as templates, other materials such as drugs or chromophores can be effortlessly embedded inside the star polymer via self-assembled occlusion complex formation. This ability coupled with the efficacy of gold nanoshells in absorbing NIR light and transferring the light energy as heat to their surrounding environment can lead to an integrated form of imaging contrast, drug-delivery system, and photothermal ablation agent. v ACKNOWLEDGEMENTS I would like to thank Dr. Melanie McNeil who has provided me an once-in-alifetime opportunity to do my thesis at IBM Almaden Research Center (ARC). I really appreciate her support, advice, and help during the time I was working on my thesis and master's program at SJSU. I would also like to thank Dr. Joseph Sly for being a wonderful advisor whom I would be forever in-debt for what he has done for me during my tenure at IBM ARC. This included but not limited to his tremendous help, support, and his awe-inspiring knowledge that he willingly shared with me. I would also like to acknowledge great help from Victor Lee who has been an amazing lab master. My sincere gratitude goes to Dr. Robert Miller for all his great feedback and input so I could obtain the best possible results in my research. I would also like to thank Dr.