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Here, we engineer the lattices from distorted to strain\u2010graded in LnNCs by CaF<jats:sub>2<\/jats:sub> deposition on vacancy\u2010controlled \u03b2\u2010Na<jats:sub>x<\/jats:sub>GdF<jats:sub>3+x<\/jats:sub>:Yb,A (A = Tm\/Er, x = 0.5, 0.75, 1) NCs. We demonstrate that strain\u2010graded lattices with high phonon energy enhance the multi\u2010phonon orbit\u2010lattice relaxation (MPR) in the downconversion process more effectively than distorted lattices, which helps to extend the near\u2010infrared\u2010IIb (NIR\u2010IIb, 1500\u20131700\u00a0nm) lifetime of Er<jats:sup>3+<\/jats:sup>\/Tm<jats:sup>3+<\/jats:sup> by 2\u223c4 times. Subsequent epitaxial CaF<jats:sub>2<\/jats:sub> growth further attenuates surface phonon coupling, enabling exponential tunability of NIR\u2010IIb lifetime (Tm<jats:sup>3+<\/jats:sup>: 0.74\u223c6.28\u00a0ms; Er<jats:sup>3+<\/jats:sup>: 0.055\u223c9.2\u00a0ms). Finally, we showcase the potential of these LnNCs in time\u2010resolved multiplexed bioimaging.<\/jats:p>","DOI":"10.1002\/anie.202513988","type":"journal-article","created":{"date-parts":[[2025,8,25]],"date-time":"2025-08-25T09:52:24Z","timestamp":1756115544000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":12,"title":["Lattice\u2010Engineered Lanthanide Nanocrystals with Tunable Near\u2010Infrared\u2010IIb Lifetime"],"prefix":"10.1002","volume":"64","author":[{"given":"Feng","family":"Ren","sequence":"first","affiliation":[{"name":"CAS Key Laboratory of Nano\u2010Bio Interface Jiangsu Key Laboratory of Organoid Engineering and Precision Medicine Division of Nanobiomedicine and <i>i<\/i>\u2010Lab Suzhou Institute of Nano\u2010Tech and Nano\u2010Bionics Chinese Academy of Sciences  Suzhou 215123 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