We studied the spectral-luminescent properties of (ZrO2)0.805(Y2O3)0.188(Pr2O3)0.007 and (ZrO2)0.802(Y2O3)0.195(Pr2O3)0.003 crystals grown by directional melt crystallization in a cold skull. Analysis of the absorption spectra of the crystals suggested the presence of Pr3+ and Pr4+ ions. Measurement of the relative intensities of the luminescence bands corresponding to the 3P0 → 3H4,5, 3P0 → 3F2,3,4, 3P1 → 3H5 and 1D2 → 3H4 optical transitions of the Pr3+ ions, and analysis of luminescence extinction kinetics for the 3P0 and 1D2 levels of the Pr3+ ions, suggests the presence of cross-relaxation (1D2 → 1G4) → (3H4 → 3F4) of the Pr3+ ions in the ZrO2-Y2O3-Pr2O3 crystals.