The polarized absorption spectra, polarized fluorescence spectra, and fluorescence decay curves of Pr3+ ions in anisotropic PbWO4 single crystal, which was grown by the modified Bridgman method, were measured at room temperature. The standard and modified Judd–Ofelt theories, extended to anisotropic crystal, have been applied to analyze the spectra. The spectroscopic parameters, including the Judd–Ofelt intensity parameters Ωt (t=2,4,6), spontaneous emission probabilities, fluorescence branching ratios, radiative lifetimes, stimulated emission cross sections, and fluorescence quantum efficiencies, were estimated. The good spectroscopic properties show the possible application of the Pr3+-doped PbWO4 crystal as solid-state and self-stimulated Raman laser materials.