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Ultrasmall and multifunctional nanoparticles are highly desirable for photothermal cancer therapy, but the synthesis of these nanoparticles remains a huge challenge. Here, we used a dendrimer as a template to synthesize ultrasmall photothermal agents and further modified them with multifunctional groups. Dendrimer-encapsulated nanoparticles (DENPs) including copper sulfide, platinum, and palladium nanoparticles possessed a sub-5 nm size and exhibited an excellent photothermal effect. DENPs were further modified with TAT or RGD peptides to facilitate their cellular uptake and targeting delivery to tumors. They were also decorated with fluorescent probes for real-time imaging and tracking of the particles' distribution. The in vivo study revealed RGD-modified DENPs efficiently reduced the tumor growth upon near-infrared irradiation. In all, our study provides a facile and flexible scaffold to prepare ultrasmall and multifunctional photothermal agents.

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Theranostic nanoparticles that possess multiple diagnostic modalities and allow spatiotemporally controlled therapies can significantly improve therapeutic outcomes and reduce adverse effects. Here, an intelligent and biocompatible theranostic formulation is developed based on dendritic platinum–copper alloy nanoparticles (DPCN) for cancer therapy. DPCN have excellent photothermal effect, and can load anticancer drugs such as doxorubicin in their porous structure and release the loaded drugs in response to near infrared light or moderate acidic stimulus. They also inherently have multimodal imaging modalities. Upon the guidance of photoacoustic imaging, DPCN‐mediated photothermal treatment efficiently inhibits tumor growth in vivo. Furthermore, doxorubicin‐loaded DPCN completely suppress the tumor growth even under a low treatment temperature, which avoids hypothermia‐induced damage to normal tissues. Our study develops an excellent theranostic nanoparticle with inherent multimodal imaging and therapeutic modalities for chemophotothermal cancer therapy.