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et al., Nanoparticle-mediated photothermal therapy (NP-PTT) constitutes a flexible, highly selective, cost effective, and accurate tool for cancer treatment alone or in combination with other therapies such as radiotherapy or chemotherapy. The future application of NP-PTT in real life mainly depends on the design and synthesis of novel multifunctional nanoparticles that could overcome the current limitations of NP-PTT such as limited penetration depth and absence of therapy control. In this work, ultrasmall (≈2.4 nm) NdVO stoichiometric (100% constituent Nd ions) nanoparticles are reported, which are capable of in vivo sub-tissue localized heating under 808 nm optical excitation while providing, simultaneously, the possibility of high penetration near-infrared fluorescence imaging. Ultrasmall stoichiometric NdVO nanoparticles have evidenced a superior light-to-heat conversion efficiency. This is explained in terms of their large absorption cross-section at 808 nm (consequence of the particular spectroscopic properties of neodymium ions in NdVO and of the high neodymium content) as well as to their ultrasmall size that leads to large nonradiative decay rates. Results included in this work introduce ultrasmall, NdVO stoichiometric nanoparticles to the scientific community as multifunctional photothermal agents that could be considered as an alternative to traditional systems such as metallic, organic, or carbon-based nanoparticles., This project was supported by the Spanish Ministerio de Economía y Competitividad under project and MAT2013-47395-C4-1-R. The authors acknowledge support from Instituto de Salud Carlos III (FIS, PI15/00974) and Comunidad Autónoma de Madrid (CAM, Skin-Model, S2010/BMD-2359). B.d.R. thanks Universidad Autónoma de Madrid for an FPI grant. D.J. and M.D.D. acknowledge fi nancial support of the Ministry of Education, Science, and Technological development of the Republic of Serbia (grant number 45020). G.D. acknowledges the fi nancial support of the Slovenian Research Agency (ARRS) through program no. P2-0148 and project J2-6754. The authors thank COST action CM1403.