The potential of gold nanoparticles (GNPs) in therapeutic and diagnostic cancer applications is becoming increasingly recognized. These biologically compatible particles can be easily synthesized, tuned to different sizes, and functionalized by conjugation to various biologically useful materials. Efficient and specific delivery to tumor tissue can then be accomplished either by passive accumulation in leaky tumor vessels and tissue, or by directly targeting tumor-specific biomarkers. Tumor-localized GNPs can serve as both adjuvants for enhancing the efficacy of radiation therapy and also as contrast agents for various imaging modalities. In this review, we will discuss recent advancements and future potential in the application of GNP as both a radiosensitizer and an imaging contrast agent. Due to their versatility and biocompatibility, gold nanoparticles may represent a novel theranostic adjuvant for radiation applications in cancer management.