Optical spectra of Dy3+:LiYF4 (Dy3+:YLF) single crystal were analyzed using Judd–Ofelt theory and discrete variational multielectron method (DVME). Oscillator strengths (OS) of transitions up to 39000cm−1 in the absorption spectrum, branching ratios and nonradiative transition rates were calculated; assignment of the absorption transitions was given. A good agreement between calculated and experimental values of branching ratios for transitions from quartet 4F(3)9/2 to the low-lying sextet levels is demonstrated. Ab initio calculations of OS were performed.