LaOI:Yb 3+ /Er 3+ nanostructures, including nanofibers and nanobelts, were successfully synthesized by electrospinning combined with a double-crucible iodination method using NH 4 I as the iodine source. X-ray diffraction (XRD) analysis reveals that LaOI:Yb 3+ /Er 3+ nanostructures are tetragonal in structure with a space group of P4/nmm. Scanning electron microscopy (SEM) analysis shows that the diameter of LaOI:Yb 3+ /Er 3+ nanofibers and the width and thickness of LaOI:Yb 3+ /Er 3+ nanobelts are 147.48 ± 17.50 nm, 1.95 ± 0.20 μm and 350 nm, respectively, under the 95% confidence level. Up-conversion (UC) emission spectroscopy analysis shows that LaOI:Yb 3+ /Er 3+ nanostructures emit strong green and red up-conversion emission centered at 523 nm, 540 nm and 667 nm under the excitation of a 980 nm diode laser (DL), which are attributed to 2 H 11/2 → 4 I 15/2 , 4 S 3/2 → 4 I 15/2 and 4 F 9/2 → 4 I l5/2 energy level transitions of Er 3+ , respectively. It is found that the relative intensities of green and red emission vary obviously by changing the molar concentration of Er 3+ ions, and the optimum molar ratio of Yb 3+ to Er 3+ is 10 : 5 in the as-prepared LaOI:Yb 3+ /Er 3+ nanofibers. The possible formation mechanisms of LaOI:Yb 3+ /Er 3+ nanofibers and nanobelts are also proposed.