The homogeneity of deuterium distribution in potassium dideuterium phosphate single crystals was studied by Raman and infrared spectroscopy analyses. Results indicated that the pyramidal section exhibited more homogeneous deuterium distribution than the prismatic section. Supersaturation slightly affected the deuterium homogeneity in the pyramidal section of crystals grown rapidly from 80% deuterated solution. Deuterium homogeneity in the prismatic section decreased with increasing supersaturation level of the growth solution.