Traditional therapy for cancer is subject to some evident obstacles, including low effectiveness, resistance, systemic complication, etc. Gold nanostructures responsive to near-infrared (NIR) light are attractive for non-invasive and targeted therapy because of their unique physical properties especially strong absorption and scattering, and high surface area-to-volume ratio as well as the ease of which their surface chemistry can be manipulated to enhance biocompatibility surface modification and functionalization. In this Review, the progress of photothermal therapy (PTT) as well as the targeted delivery of anticancer agents as the predominant applications of gold nanostructures is detailed, with a focus on imaging-guided therapy and optimizing operational parameters. The NIR light-controlled targeted delivery and/or photothermal ablation of gold nanostructures in the treatment of metastasis are also briefly discussed. These gold nanostructures pave the way for developing better therapeutic strategies of cancer.