Lanthanide-doped upconversion nanoparticles (UCNPs) have significant applications for single-molecule probes and high-resolution display. However, one of their major hurdles is the weak luminescence, and this remains a grand challenge to achieve at the single-particle level. Here, 484-fold luminescence enhancement in LuF 3 :Yb 3+ , Er 3+ rhombic flake UCNPs is achieved, thanks to the Yb 3+ -mediated local photothermal effect, and their original morphology, size, and good dispersibility are well preserved. These data show that the surface atomic structure of UCNPs as well as transfer from amorphous to ordered crystal structure is modulated by making use of the local photothermal conversion that is generated by the directional absorption of 980 nm light by Yb 3+ ions. The confocal luminescence images obtained by superresolution stimulated emission depletion also show the great enhancement of individual LuF 3 :Yb 3+ , Er 3+ nanoparticles; the high signal-to-noise ratio images indicate that the laser treatment technology opens the door for single particle imaging and practical application.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adfm.201906137. studies obtained in the last decades are performed by a cluster of nanoparticles, which is quite different from that of an individual particle. [9,10] Research by Haro-González and co-workers demonstrates that the total fluorescence intensity of nanoparticle group not only depends on the number of particles, but also on the direction of the excitation polarization and the orientation of the UCNPs. [11] Unfortunately, a major obstacle for practical application of UCNPs at single particle level is still their weak luminescence. [12][13][14] Thus, it is necessary to find a useful strategy to optimize the optical properties of individual up-conversion nanoparticle (UCNP) for better luminescence efficiency.Complicated surface states of UCNPs play an important role in their upconversion efficiency, in which majority atoms combine with the enriched surface defects, leading a serious surface quenching effect. [15][16][17] To date, many surface passivation strategies, [18] like annealing treatment [17,19] and coating technology, [20,21] have been proposed for improving upconversion luminescence (UCL), however most of these efforts may not necessarily lead to the optimal enhancement at the single-particle level. This is because 1) annealing treatment can cause agglomeration of UCNPs and 2) the use of coreshell configuration is difficult to achieve in 1D and 2D core UCNPs. Thus, it is urgent to find a useful strategy that can not only efficiently passivate surface defects, but also maintain the good uniformity of particle size, morphology, and the excellent dispersibility.In this work, Yb 3+ -/Er 3+ -codoped LuF 3 UCNPs were synthesized by co-precipitation method, and irradiated by high-energy near-infrared (NIR) laser ( Figure S2, Supporting Information). Here, we propose photothermal conversion in the local lattice ...