The Cr2+ doped CdS0.8Se0.2 crystals were grown by the vertical, self-seeded, physical vapor transport (PVT) technique. Good quality, crack- and inclusion-free single crystals were grown with an average Cr2+ concentration of 5 × 1018 cm−3. Different source-to-tip distances were used to improve the segregation coefficient (Crcrystal/Crsource) of the grown crystals. It was observed that lowering the source-to-tip distance increases the segregation coefficient dramatically. With a 2-cm source-to-tip distance, good quality crystals were grown with uniform Cr2+ concentration throughout the ingot. The segregation coefficient was found to be ∼0.85. The composition of the crystals was also found to be fairly uniform along the length and across the diameter.