The development and optimization of near-infrared (NIR)-absorbing nanoparticles for use as photothermal cancer therapeutic agents has been ongoing. This work exploits the properties of gold/gold sulfide NIR-absorbing nanoparticles (≈35–55 nm) that provide higher absorption (98% absorption and 2% scattering for gold/gold sulfide versus 70% absorption and 30% scattering for gold/silica nanoshells) as well as potentially better tumor penetration. The ability to ablate tumor cells in vitro and efficacy for photothermal cancer therapy is demonstrated, and an in vivo model shows significantly increased long-term, tumor-free survival. Furthermore, enhanced circulation and biodistribution is observed in vivo. This class of NIR-absorbing nanoparticles has the potential to improve upon photothermal tumor ablation for cancer therapy.