The complexity associated with advanced cancer disease necessitates repeated administration of radio / chemotherapy primarily due to recurrent disease and sub-optimal drug delivery. Combination therapies have emerged as powerful alternatives to ‘single-agent therapies' since they enhance cell death typically by overcoming multiple cell-death resistance mechanisms in cancer cells. We describe the design and generation of nanoscale architectures based on gold nanorods for delivering combination treatments selectively to cancer cells. Multisegmented gold nanorods with spatially defined regions for cancer cell targeting, combination treatment, and optical (near infrared, NIR) imaging were designed and generated using electrochemical synthesis techniques. These nanorods have significant advantages over commonly used nanoparticles due to the ability to dedicate specific regions at the nanoscale to biological function (i.e. targeting, cell ablation, and optical imaging). Related to this, we describe a newly developed method for the high throughput generation of gold nanorods using a templated electrodeposition approach with an eye towards increasing the yield of nanorods. The uptake, cytotoxic efficacy, selectivity, and mechanisms of cell death induced upon chemotherapeutic drug delivery using multisegmented gold nanorods were evaluated with chemoresistant human prostate cancer cell lines. It is anticipated that these nanorod architectures will have significant impact on the delivery of combination treatments for advanced cancer disease.