Rational design and preparation of multifunctional low dimensional nanomaterials are of great importance for in vivo imaging and safety therapy. Meanwhile, nanomaterials with good bio-compatible and effectively photothermal conversion are still demanded to be fabricated in biomedicine. In this work, we have developed two-dimensional bismuth selenide nanosheets as the imaging and photothermal nanoagents. Through doping engineering, the near infrared photothermal conversion of Nd doped nanosheets was boosted by 52 %, which is higher than many previous works. Besides, the prepared nanomaterials can realize infrared and in vivo computed X-ray tomography bioimaging, due to the rich optical-magnetic properties of Nd atoms. The in vitro and vivo experiments with mice display that the Nd doped nanosheets have low toxicity and high biocompatibility. More importantly, the nanomaterials can efficiently achieve photothermal tumor ablation. It is suggested that designed and developed nanosheets have promising applications for biomedicine.