Phototherapy, including photothermal therapy (PTT)/photodynamic therapy (PDT), is usually considered as a promising strategy for cancer treatment due to its noninvasive and selective therapeutic effect by laser irradiation. A light-activatable nanoplatform based on bovine serum albumin (BSA)-coated Bi2Te3 nanosheets conjugated with methylene blue (MB) was successfully designed and constructed for bimodal PTT/PDT combination therapy. The resultant nanoconstruct (BSA-Bi2Te3/MB) exhibited high stability in various physiological solutions and excellent biocompatibility. Especially, the nanoconstruct not only possessed strong near-infrared absorption and high photothermal conversion as a photothermal agent for efficient tumor ablation but also could successfully load photosensitizer for PDT of tumor. When exposed to laser irradiation, tumors in mice with BSA-Bi2Te3/MB injection were completely eliminated without recurrence within 15 d, demonstrating the potential of the nanoconstruct as a bimodal PTT/PDT therapeutic platform for cancer treatment.