8231wileyonlinelibrary.com the tumor, many kinds of nanomaterials have been developed for the imaging of tumor, such as magnetic (Fe [2] /Gd [3] /Mn [4] based) nanoparticles for magnetic resonance imaging (MRI), luminescent (such as lanthanide [5] /carbon [6] -based) nanoparticles for fluorescent imaging, and high atomic number or high X-ray attenuation coefficient nanomaterials (iodine [7] /gold [8] / bismuth [9] -based) for X-ray computed tomography (CT) imaging. Furthermore, to cure the tumor, various nanomaterials have also been investigated for developing new therapy methods, including nanocarriers (mesoporous silica, [10] polymer nanocapsules [11] ) for advanced chemotherapy, nanophotosensitizers [12] for the photodynamic therapy and photothermal nanoagents for the ablation of tumor. Among these therapy methods, near-infrared (NIR) laser-induced photothermal ablation therapy (PAT) has drawn much attention as a minimally-invasive and potentially more effective technology. [12b,13] For achieving the NIR-PAT for tumors, several types of photothermal nanoagents have been well researched, containing polymer [14] /metal [15] /carbon [6] / semiconductor [16] -based nanomaterials. Our group has also prepared Cu [16a,17] /W [16b,18] -based semiconductors as novel and efficient photothermal agents. To further enhance the therapy efficiency and minimize side effects from NIR-PAT, the combination of NIR-PAT with bioimaging has been proposed for the simultaneous diagnosis and therapy of tumors, since bioimaging in vivo can be used to guide the design of NIR-PAT plans, for example, by choosing the optical doses and/or optimal irradiation region, and deciding the best timing of laser treatment when the photothermal agent reaches the peaked accumulation in the targeted lesion. [19] For realizing the imaging-guided NIR-PAT, multifunctional nanomaterials, which contain NIR photothermal conversion ability and at least one of bioimaging functions, should be designed and prepared. Currently, three kinds of multifunctional nanomaterials with complex structures have been chiefly developed. The first kind is the mixture containing two or more imaging/therapy agents that are encapsulated/conjugated by organic/polymer molecules, including metal-metal, [3,20] The ideal theranostic nanoplatform for tumors is a single nanoparticle that has a single semiconductor or metal component and contains all multimodel imaging and therapy abilities. The design and preparation of such a nanoparticle remains a serious challenge. Here, with FeS 2 as a model of a semiconductor, the tuning of vacancy concentrations for obtaining "all-in-one" type FeS 2 nanoparticles is reported. FeS 2 nanoparticles with size of ≈30 nm have decreased photoabsorption intensity from the visible to near-infrared (NIR) region, due to a low S vacancy concentration. By tuning their shape/size and then enhancing the S vacancy concentration, the photoabsorption intensity of FeS 2 nanoparticles with size of ≈350 nm (FeS 2 -350) goes up with the increase of the wavelength...