Inorganic phosphors that emit near-infrared (NIR) light are highly valued as fluorescent probes for in vivo imaging of biological tissue. NIR-imaging, however, is limited by the paucity of probes that emit over the NIR-II window (1000–1400 nm). We are interested in exploring the potential of double-layered perovskite structures harboring lanthanide ions as NIR-II fluorescent probes. In this report, we describe the synthesis, and characterization of the photoluminescence, afterglow and thermo-luminescence of Nd
3+-doped Sr
3Sn
2O
7 together with an analysis of its structural properties. Sr
3Sn
2O
7:Nd
3+ has a double-layered perovskite structure with oxygen octahedral tilt and rotation, which leads to an intense NIR-II luminescence from 4
f–4
f transition in Nd
3+ ions; the intensity of NIR-II photoluminescence of Sr
3Sn
2O
7:Nd
3+ is 10
2 times higher than that of an ordinary perovskite structure, namely SrSnO
3:Nd
3+. Moreover, we show the intra-layer planar defect in Sr
3Sn
2O
7:Nd
3+ contributes to the long-lived NIR-II afterglow. Finally, we show time-resolved imaging of the long-lived NIR-II fluorescence of Sr
3Sn
2O
7:Nd
3+ generate high-contrast images of probes embedded within a model tissue.
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