The axial Fe3+ center Fe1 with the crystal field parameter b20≈3130×10−4cm−1 is well studied in congruent lithium tantalate crystals. The second axial Fe3+ center Fe2 was discovered and investigated by the electron paramagnetic resonance in stoichiometric samples prepared by vapor transport equilibrium treatment. The crystal field parameter of the Fe2 center (b20≈2050×10−4cm−1) is significantly smaller than for Fe1. The electron nuclear double resonance measurements have shown that hyperfine interactions of the Fe3+ electrons with the surrounding Li nuclei for Fe2 are stronger than for Fe1. Therefore, the conclusion was made that in the case of Fe2 center the iron ion substitutes for Ta and has Li nuclei in the nearest neighborhood, whereas in the case of Fe1 center it substitutes for Li, has Ta nuclei as nearest neighbors and Li nuclei in the second shell only.