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Core-shell structure is an obvious concept to suppress surface-related deactivations in lanthanide-doped upconversion nanoparticles (UCNPs). However, no direct observation of atomic-scale surface restoration, which can improve the upconversion photoluminescence, has been reported. Here, we use aberration-corrected high-angle annular dark field scanning transmission electron microscopy to study the surface condition of KLu 2 F 7 :Yb 3+ ,Er 3+ bare core UCNPs. Due to the very thin and uniform thickness of the UCNPs, we observe unambiguously that the recovery from surface defects enhances upconversion photoluminescence. Furthermore, the realization of dominant green lasing emission under pulsed laser excitation confirms the high crystallinity of the UCNPs.