Near-infrared (NIR) light-induced photothermal cancer therapy using nanomaterials as photothermal agents has attracted considerable research interest over the past few years. As the key factor in photothermal therapy systems, a variety of photothermal agents have been developed. However, the exploration of novel photothermal therapy nanoplatforms with high NIR absorption remains a significant challenge, especially those working in both NIR-I and NIR-II windows. In this work, Bi19S27I3 nanorods with remarkably high absorption covering the whole visible light to the entire NIR-I and NIR-II regions have been successfully prepared through a facile solvothermal approach. The as-synthesized Bi19S27I3 nanorods have a high photothermal conversion efficiency of 42.7% at 808 nm (NIR-I) and 41.5% at 1064 nm (NIR-II), making them a promising candidate for photothermal therapy. In vitro cell viability assay reveals that the Bi19S27I3 sample has good biocompatibility and exhibits significant cell-killing effect under NIR irradiation. In vivo anti-tumor experiments demonstrate that the tumor growth can be effectively inhibited by fatal hyperthermia ablation mediated by Bi19S27I3 nanorods under the irradiation of an 808 nm or 1064 nm laser. Therefore, this study should be primarily beneficial for the development of new materials for NIR photothermal therapy applications.