Traditional oncology treatment modalities are often associated with a poor therapeutic index. This has driven the development of new targeted treatment modalities, including several based on the conversion of optical light into heat energy (photothermal therapy, PTT) and sound waves (photoacoustic imaging, PA) that can be applied locally. These approaches are especially effective when combined with photoactive nanoparticles that preferentially accumulate in tissues of interest and thereby further increase spatiotemporal resolution. In this study, two clinically used materials that have proven effective in both PTT and PA-indocyanine green (ICG) and gold nanoparticles (AuNPs)-are combined into a single nanoformulation. These particles, "ICG-AuNP clusters," incorporate high concentrations of both moieties without the need for additional stabilizing or solubilizing reagents. The clusters demonstrate high theranostic efficacy both in vitro and in vivo, compared with ICG alone. Specifically, in an orthotopic mouse model of triple-negative breast cancer, ICG-AuNP clusters can be injected intravenously, imaged in the tumor by PA, and then combined with near-infrared laser irradiation to successfully thermally ablate tumors and prolong animal survival. Altogether, this novel nanomaterial demonstrates excellent therapeutic potential for integrated treatment and imaging.