CaF2:Ho3+/Yb3+nano-particleswithintensegreenup-conversion(UC)luminescencearesuccessfullysynthesizedviaafacilehydrothermalapproachbyusingNH4FasthefluoridesourceandNa2EDTAasachelatingreagent.PowderXraydiffraction(XRD),transmissionelectronmicroscopy(TEM),fieldemissionscanningelectronmicroscopy(FE-SEM),andUCemissionspectraareusedtocharacterizethestructures,shapes,andluminescentpropertiesofthesamples.TheeffectsfromfluoridesourcesandchelatingreagentsontheformationsofCaF2nano-particlesareinvestigated,andtheformationprocessisalsodeduced.Undertheexcitationofa980-nmlaserdiode,thesampleseachshowagreenup-conversionemissioncenteredat540nmcorrespondingtothe5S2/5F4→5I8transitionsofHo3+.Moreover,theUCmechanismsofHo3+/Yb3+co-dopedCaF2nano-particlesarealsodiscussed.