The ability of near-infrared (NIR) light to penetrate tissues deeply and to target malignant sites with high specificity via precise temporal and spatial control of light illumination makes it useful for diagnosing and treating diseases. Owing to their unique biocompatibility, surface chemistry and optical properties, gold nanostructures offer advantages as in vivo NIR photosensitizers. This chapter describes the recent progress in the varied use of NIR-resonant gold nanostructures for NIR-light-mediated diagnostic and therapeutic applications. We begin by describing the unique biological, chemical and physical properties of gold nanostructures that make them excellent candidates for biomedical applications. From here, we make an account of the basic principles involved in the diagnostic and therapeutic applications where gold nanostructures have set foot. Finally, we review recent developments in the fabrication and use of diverse NIR-resonant gold nanostructures for cancer imaging and cancer therapy.