Abstract Single crystals of Mn 1‐x Fe x In 2 Se 4 with 0 ≤ x ≤ 1.0 were grown by chemical vapor transport technique using I 2 as transporting agent. The resulting crystals appeared as brilliant black plates. X‐ray powder diffraction data could be indexed following the hexagonal structure with space group R $ \bar 3 $ m for the low Fe concentration samples, while the high concentration sample is associated to the space group P6 3 mc. Both polytypes have similar parameters, however the c parameter reduces as the Fe concentration increases, therefore the number of anion slabs decreases. The characterization of the crystals was based on morphological observations and optical absorption as a function of temperature. The obtained energy gap for the samples at different Fe concentrations suggested that they behave as direct energy gap semiconductors. (© 2005 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)